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Selective variegated methylation of the p15/INK4B CpG island is a high frequency event in acute myeloid leukemia (AML) Item Type text; Dissertation-Reproduction (electronic) Authors Dodge, Jonathan Eldon Publisher The University of Arizona. Rights Copyright © is held by the author. Digital access to this material is made possible by the University Libraries, University of Arizona. Further transmission, reproduction or presentation (such as public display or performance) of protected items is prohibited except with permission of the author. Download date 27/05/2018 16:25:32 Link to Item http://hdl.handle.net/10150/284143

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Selective variegated methylation of thep15/INK4B CpG island is a high frequency

event in acute myeloid leukemia (AML)

Item Type text; Dissertation-Reproduction (electronic)

Authors Dodge, Jonathan Eldon

Publisher The University of Arizona.

Rights Copyright © is held by the author. Digital access to this materialis made possible by the University Libraries, University of Arizona.Further transmission, reproduction or presentation (such aspublic display or performance) of protected items is prohibitedexcept with permission of the author.

Download date 27/05/2018 16:25:32

Link to Item http://hdl.handle.net/10150/284143

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SELECTIVE VARIEGATED METHYLATION OF THE pl5/INK4B CPG ISLAND IS A HIGH FREQUENCY EVENT IN

ACUTE MYELOID LEUKEMIA (AML)

by

Jonathan Eldon Dodge

A Dissertation Submitted to the Faculty of the

COMMITTEE ON PHARMACOLOGY AND TOXICOLOGY (GRADUATE)

In Partial Fulfillment of the Requirements for the Degree of

DOCTOR OF PHILOSOPHY

In the Graduate College

THE UNIVERSITY OF ARIZONA

2 0 0 0

UMI Number 9972079

<S>

UMI UMI Microfomi9972079

Copyright 2000 by Bell & Howell Information and Learning Company. All rights reserved. This microform edition is protected against

unauthorized copying under Title 17, United States Code.

Bell & Howell Information and teaming Company 300 North Zeeb Road

P.O. Box 1346 Ann Arbor, Ml 48106-1346

2

THE UNIVERSITY OF ARIZONA ® GRADUATE COLLEGE

As members of the Final Examination Committee, we certify that ve have

read the dissertation prepared by Jonathan Eldon Dodge

entitled Selective variegated methylation of the pl5/INK4B CpG island

is a high frequency cMcnt- in acute raveloid leukemia fAMT.">

and recommend that it be accepted as fulfilling the dissertation

requirement for the Degree of Doctor of Philosophy

G. Tim BQii^eAo^ Plj.D. Date

Bernard W. Futscher, Ph.D.

Charl^rte^McQueen,

/ Date

U.~( C -C2£^ (y

Qin Chen, P^D. Date

I. Gle^m Sipes, Ph.D. ^C2Si.

Date

Final approval and acceptance of this dissertation is contingent upon the candidate's submission of the final copy of the dissertation to the Graduate College.

I hereby certify that I have read this dissertation prepared under my direction and recommend that it be accepted as fulfilling the dissertation requirement.

Dissertation Director Bernard W. Futscher, Ph.D.

4/14- /oi Date

3

STATEMENT BY AUTHOR

This dissertation has been submitted in partial Fulfillment of requirements for an advanced degree at The University of Arizona and is deposited in the University Library to be made available to borrowers under rules of the Library.

Brief quotations from this dissertation are allowable without special permission, provided that accurate acknowledgment of source is made. Requests for permission for extended quotation from or reproduction of this manuscript in whole or in part may be granted by the head of the major department or the Dean of the Graduate College when in his or her judgment the proposed use of the material is in the interests of scholoarship. In all other instances, however, permission must be obtained from the author.

4

ACKNOWLE DGMENTS

A number of people made significant contributions to this work. Of particular importance are: (1) intellectual and technical contributions, and (2) financial support of my graduate education.

In the first category, the studies originally done by Dr. James G. Herman at Johns Hopkins University provided us with the initial observation of pl5 methylation in AML that stimulated our sequence of studies. Also at Johns Hopkins, Dr. Elizabeth Cameron, a then graduate student in Dr. Stephen B. Baylin's lab helped us establish a protocol for pl5 mRNA detection. An important technical advance was provided by Dr. Vaillancourt's lab, at the University of Arizona, with the their help a pl5 fusion protein was generated and used to establish a protocol for pl5 protein detection. I was fortunate to learn sodium bisulfite sequencing from my advisor Dr. Bernard W. Futscher and then graduate student Dr. George S. Watts. In addition, the studies of pl5 and pl6 introduction into Jurkat were greatly aided by the use of microarray technology developed in Dr. Futscher's lab by current postdoc Dr. George S. Watts. Intellectually, I was helped by my adivsor Dr. Futscher as well as my committee members Dr. Charlene McQueen, Dr. Qin Chen, Dr. G. Tim Bowden, and Dr. I Glenn Sipes.

As a graduate student I was supported financially by: (1) the University of Arizona Graduate College Fellowship in my first year, (2) the Robert S. Flinn Center for Toxicology Fellowship for two years, (3) an NIEHS Center for Toxicology Trainee Grant for two years, and (4) an American Foundation for Pharmaceutical Education (AFPE) Fellowship for three years. These means of support were tremendously helpful and demonstrate the strength of the Pharmacology and Toxicology Department at the University of Arizona.

This work is dedicated to my father and mother, Michael

and Christine Dodge, my brother, Stephen Dodge, and my

sister, Catherine Dodge. They all supported my desire to

understand the world around me.

6

TABLE OF CONTENTS

LIST OF FIGURES 9 LIST OF TABLES 11 LIST OF ABBREVIATIONS 12 ABSTRACT 13

CHAPTER 1 - INTRODUCTION 15 Overview of S-methylcytosine in marranalian cells. . . 15 Dysregulation of 5-methylcytosine in human cancer involves the inactivation of genes 21 Loss of deoxycytidine kinase (dCK) is implicated in drug resistance and dCK is a candidate for inactivation by DNA methylation 23 Potential role of pl5 and pl6 in human cancer. ... 24 Statement of purpose of the present studies 30

CHAPTER 2 - MATERIALS AND METHODS 33 Cell culture 33 Normal cells and patient samples obtained for use in this study 34 DNA isolation and Southern blot analysis 34 RNA isolation and Northern blot analysis 36 Reverse-transcriptase polymerase chain reaction (RT-PCR) 36 Generation of pl5 mRNA by in vitro transcription for use as a positive control 38 Protein isolation and Western blot 39 Generation of pl5 recombinant protein for use as a positive control 40 Isolation of DNA and bisulfite sequencing of dCK, pl5, and pl6 41 Transient transfection with CAT gene reporter constructs 43 Selection of stable expression of pl5 and pl6 in cell lines 43 TGF-I3, PMA, PMA/Ionomycin, cytosine arabinoside, and daunorubicin treatment of cell cultures 45 MTS assay for drug sensitivity 46 FACS analysis of cell cycle by propidium iodide staining, FACS analysis of apoptosis by Annexin V/PI staining, and cell growth in liquid culture 46 Microarray expression analysis 46

7

TABLE OF CONTENTS - Continued

CHAPTER 3 - DETERMINATION OF 5-METHYLCYTOSINE INFLUENCE ON dCK EXPRESSION 51

Drug-sensitive and -resistant model cell lines. . . .51 dCK gene structure and expression 52 DNA methylation mapping of 5' dCK CpG island in model cell lines, normal human peripheral blood lymphocytes, and AML patient samples 58

CHAPTER 4 - DETERMINATION OF 5-METHYLCYTOSINE INFLUENCE ON P15 AND P16 EXPRESSION 64

Established human leukemia cell line models 64 pl5 and pl6 mRNA and protein studies in human leukemia cell lines 66 pl5 promoter studies with the CAT reporter gene. - .70 DNA methylation mapping of pl5 and pl6 5' CpG islands in established human leukemic cell lines, normal human bone marrow, and AML patient samples 72

CHAPTER 5 - INTRODUCTION OF P15 AND P16 PROTEINS INTO JURKAT 81

Stable overexpression of pl5 or pl6 in Jurkat I: establishment of pl5 and pl6 positive subclones. . . 81 Stable overexpression of pl5 or pl6 in Jurkat II: growth is reduced only in pl5 positive cells not pl6 positive cells, retinoblastoma phosphorylation is not constitutively altered, and sensitivity to cytosine-arabinoside, and daunorubicin is unchanged 91 Stable overexpression of pl5 or pl6 in Jurkat III: microarray gene expression analysis of 5700 genes reveals an upregulation of genes involved in cellular differentiation 97

CHAPTER 6 - DISCUSSION 103 Aberrant DNA methylation of the pl5 5' CpG island occurs in the majority of acute myeloid leukemia (AML) patients and might dysregulate normal hematopoietic differentiation 103 Aberrant methylation of pl5 as a marker of AML and potential target for novel drug therapeutic treatments 108 General potential for novel therapeutic intervention of epigenetic defects in human cancer 112

8

TABLE OF CONTENTS - Continued

APPENDIX A. SUMMARY OF STUDIES TO TEST WHETHER P15 CAN BE INDUCED IN KG-1 OR KG-la BY AGENTS NOT ASSOCIATED WITH DNA DEMETHYLATION 115

APPENDIX B. IN PREPARATION TO SUBMIT TO NUCLEIC ACIDS RESEARCH: D-HPLC AS A SIMPLE METHOD TO DETECT ABERRANT DNA METHYLATION 121

REFERENCES 125

9

LIST OF FIGURES

1, Genomic organization of the INK/ARF locus along chromosome 9p21 encoding pl5, pl9ARF, and pl6. . . .27

2, pl5 and pl6 protein homology 28

3, pl5 and pl6 functional pathway 29

4, An overview of the research presented in this dissertation 31

5, Southern blot of dCK in HL60/S, HL60/R, K562/S, and K562/R 53

6, Northern blot of dCK 55

7, Determination of cycle numbers for dCK and histone 3.3 semi-quantitative RT-PCR 56

8, Semi-quantitative RT-PCR for dCK 57

9, Biochemical basis for sodium bisulfite sequencing. .60

10, 5-methylcytosine content of dCK in leukemic model cell lines 61

11, 5-methylcytosine content of dCK in normal human tissue and AML patients 63

12, RT-PCR detection of pl5 and pl6 68

13, Western blots to detect pl5 and pl6 protein 69

14, pl5 promoter constructs with the CAT reporter gene. 71

15, 5-methylcytosine content of pl5 and pl6 in model cell lines 77

16, 5-methylcytosine content of pl5 and pl6 in normal human bone marrow and AML patients, part 1 78

17, 5-methylcytosine content of pl5 and pl6 in normal human bone marrow and AML patients, part 2 7 9

10

LIST OF FIGURES-continued

18, Individual sodium bisulfite clones of normal bone marrow and two AML patients 80

19, PGR to confirm pl5 and pl6 homozygous deletion in Jurlcat 82

20, Explanation of the tetracycline eukaryotic inducible expression system 84

21, Transient transfection of tet-GFP establishes that Tet-Off protein is functional in Jurkat Tet-off. . .85

22, Determination of inducibility of pl5 in Jurkat clones that are pl5 positive 88

23, Western blot analysis of pl5 and pl6 positive Jurkat clones 90

24, Growth of pl5 and pl6 positive Jurkat clones in liquid culture 92

25, MTS assay to determine growth of pl5 and pl6 untreated Jurkat clones 93

26, Annexin V assay for apoptotic/necrotic pl5 and pl6 positive Jurkat cells 95

27, MTS assay to determine effect of araC and daunorubicin sensitivity of pl5 and pl6 positive Jurkat cells. . 96

28, Example of 5,700 cDNA microarray analysis 99

29, Northern blots of differentially expressed genes in pl5 and pl6 positive Jurkat cells 101

30, Summary of microarray versus Northern analysis. . .102

31, Model to explain the observed methylation of pl5 but not pl6 in AML 107

32, Epigenetics/DNA methylation as a potential target of cancer pharmacology Ill

11

LIST OF TABLES

Summary of the cell lines used and tested for pl5 and pl6 mRNA by RT-PCR and pl5 and pl6 protein by immunoblots 32

Characteristics of normal human samples and human acute myeloid leukemia patients obtained for study. 62

Summary of the results obtained using a single plasmid or two separate plasmids in the tetracycline inducible expression system 89

The genes that microarray identified as differentially expressed in the pl5 or pl6 positive Jurkat cells. 100

Summary of the alterations that occur in human cancer cells 114

12

LIST OF ABBREVIATIONS

AML Acute myeloid leukemia ara-C Cytosine arabinoside ATCC American Tissue and Cell Culture 5-aza 5-azacytidine BNIP3 A bcl-2/EiP-interacting gene BSA Bovine serum albumin CAT Chloramphenicol acetyltransferase CDK Cyclin-dependent kinase CpG Cytosine-phosphate-guanosine dinucleotide dCK Deoxycytidine kinase DMEM Dulbecco's modified Eagle's mediiom DOX Doxycycline FACS Flow-assisted cell sorting FBS Fetal bovine serum G418 Neomycin GAPDH Glyceraldehype dehydrogenase GFP Green fluorescent protein HB-EGF Heparin-binding epidermal growth factor Hygro Hygromycin IMEM Iscove's modified Eagle's medium INK4 Inhibitor of cyclin-dependent kinase 4 IRF-1 Interferon-regulatory factor-1 MCLl A gene in the bcl-2 family member MyoD A gene involved in muscle differentiation NBM Normal human bone marrow PAGE Polyacrilimide gel electrophoresis PBL Peripheral blood lymphocytes PBS Phosphate buffered saline PCR Polymerase chain reaction PI Propidium iodide PMA Phorbol-13-myristate acetate PTPNl Protein tyrosine phosphatase RT-PCR Reverse-transcriptase polymerase chain

reaction T-ALL T-cell lymphoblastic leukemia TET Tetracycline TGF-P Transforming growth factor-beta TRE Tetracycline-responsive element

13

ABSTFIACT

We attempted to define target genes that were

inactivated in acute myeloid leukemia (AML) by DNA

methylation. We hypothesized that hypermethylation of 5'

CpG islands is associated with transcriptional silencing of

the corresponding gene and participates in either the

emergence of drug resistance or the conversion of normal

cells to cancer cells. To test this hypothesis the DNA

methylation status of the 5' CpG islands of dCK containing

4 9 CpGs, pl5 containing 80 CpGs, and pi 6 containing 53 CpGs

was determined by sodium bisulfite sequencing of normal

human peripheral blood lymphocytes (PBL) and bone marrow

(NBM), human leukemia cell lines, and cytosine-arabinoside

(ara-C)-resistant adult acute myeloid leukemia (AML)

patients. In PBL and NBM dCK, pl5, and pl6 were all

unmethylated. dCK was unmethylated in the paired ara-C-

sensitive (/S) ara-C-resistant (/R) leukemia cell lines

HL60/S & /R and K562/S & /R, and in the 8 AML patients

analyzed. pl6 was unmethylated in KG-1 and KG-la and both

had detectable pl6 mRNA and protein. None of the 8 AML

patients had aberrant methylation of pl€. For pl5, a

variegated pattern of aberrant methylatlon was found in KG-

1, and complete methylation of pl5 was found in KG-la. The

14

variegated pattern of pl5 methylation seen in KG-1 and the

complete methylation seen in KG-la were both associated

with no detectable pl5 mRNA or protein. pl5 was aberrantly

methylated in 6 of the 8 AML patients, 5 had a variegated

pattern of methylation, and 1 showed complete methylation.

We next introduced ectopic pl5 and pl6 into the pl5 and pl6

negative human T-cell lymphocytic leukemia cell line

Jurkat. The pl5 positive clones grew at a slower rate than

the parent cell or pl6 positive clones as measured by

growth in liquid culture and MTS assay. cDNA microarray

expression analysis differentiated pl5 and pl6 positive

subclones from the parent cell line but not from each

other. This suggests that despite the selective

methylation of pl5 but not pl6 in AML, pl5 and pl6 are

functionally similar.

15

CBASTBR 1 - ZHTRODnCTZON

Ovarvittw of 5-atttiiylcytosi.n* xn •••••• 1i.an cttlls

Genetic change is central to many human pathologies,

however, all human disease is not explained by genetic

change. The remaining changes, those changes that are

heritable and not mediated by a change in DNA nucleotide

sequence, are considered epigenetic changes. The

modification of cytosine to 5-methylcytosine, synonymous

with DNA methylation, is an epigenetic change because it is

heritable but does not have any effect on the triplet amino

acid code contained in DNA.

DNA methylation is the only tolerated modification of

cytosine, guanosine, adenine, and thymine, the four bases

that comprise DNA. Plants, mammals, and fungi methylate a

small percentage of cytosines in their DNA, but the model

organisms yeast, C. elegans, and drosophila lack 5-

methylcytosine (Riggs and Porter 1996). After first

reviewing the enzymatic maintenance of 5-methylcytosine,

the role of 5-methylcytosine in mammalian cell development,

cell differentiation, gene expression, X-chromosome

inactivation, and repression of retroviral sequences will

be discussed.

16

The enzymatic regulation of 5-methylcytosine is not

completely understood. Empirical data support a post-

replication addition of a methyl group to the 5 position of

cytosines located in 5'-CG-3' dinucleotides (Wigler 1980,

Bestor 1996). Evidence supports the almost exclusive

methylation of cytosine located 5' to guanines (Bestor

1996). These 5'-CG-3' are depleted in mammalian genomes

but tend to cluster at the 5' end of genes. These regions

of high 5'-CG-3' density located at the 5' region of genes

are referred to as "CpG islands" that are normally

unmethylated. As defined by Gardiner-Gardner and Frommer

(1987), CpG islands (1) contain > 3 times the normal

density of 5'-CG-3' dinucleotides, (2) are > 200 base pairs

in length, and (3) are located near the transcription start

site of a gene. The first mammalian DNA methyltransferase

discovered, DNMTl, adds a methyl group, using S-

adenosylmethionine (SAM) as a cofactor, to the 5 position

of cytosines in 5'-CG-3' sites. The preferred substrate of

DMNTl is hemi-methylated DNA. Recently, 3 new DNA

methyltransferases have been discovered, DNMT 2, 3a, and 3b

(Okano et al 1998). It is speculated that DNMT 3a and 3b

are de novo methylases, capable of methylating previously

unmethylated regions of DNA. In addition there has long

17

been speculation that an active DNA demethylation process

converts 5-methylcytosine to cytosine independent of DNA

replication. While several reports have been presented

that claim to have found an enzyme with DNA demethylation

activity, some have been retracted and this is still a

controversial area. Bhattacharya et al 1999 has recently

reported an active demethylation activity, but it remains

to be confirmed by other labs.

DNA methylation is implicated in mammalian

development. Mutation of DNMT 1 in mice resulted in

embryonic lethality providing direct evidence for an

essential role of DNA methylation in development (Li et al

1992). This result removed any speculation that 5-

methylcytosine had only a vestigial presence in the

mammalian genome. It has recently been founhd that

knocking out DNMT 3a or 3b (but not DNMT 2) in the mouse

also resulted in embryonic lethality (Okano et al 1999).

Complementing the mouse transgenic experiments, changes in

5-methylcytosine patterns and levels have been observed

during mouse development (Rougier et al 1998). Thus,

direct evidence shows that 5-methylcytosine regulation is

essential to mammalian development.

18

It has also been found that DNA methyiation influences

cellular differentiation. The studies reported in 197 9 by

Taylor and Jones found that the compound 5-azacytidine

resulted in phenotypic alterations in mouse cells lines.

The mechanism of 5-azacytidine's effect on differentiation

was shown to be mediated, at least in part, by inhibition

of DNA methyiation. The altered phenotypes, observed when

Swiss 3T3 or lOTl/2 mouse cells became striated muscle

cells, adipocytes, or chondrocytes, was found to be

associated with an inhibition in the normal methyiation of

DNA. Specifically, in the case of differentiation into

striated muscle cells it was found that the gene MyoDl, a

gene involved in muscle differentiation, was demethylated

by 5-azacytidine and this demethylation was associated with

MyoD transcription (Jones 1985). The discovery of 5-

azacytidine provided a useful pharmacological link between

DNA methyiation and gene transcription.

In 1975 Holliday and Pugh were one of the first to

speculate that DNA methyiation had a direct role in gene

activity. Numerous studies since 197 5 have confirmed that

the presence of DNA methyiation in the 5' CpG islands of

genes is associated with a loss of gene transcription (Bird

1986, Razin and Riggs 1980). One of the earliest studies

19

of a specific gene focused on metallothionein. It was show

that DNA methylation was not only associated with a lack of

metallothionein expression, but heavy metals such as

cadmium did not result in the expected induction of

metallothionein when DNA methylation was present (Compere

and Palmiter 1981). In summary, it is generally believed

that DNA methylation of the 5' proximal CpG islands of

genes is associated with transcriptional silencing of the

corresponding gene.

DNA methylation is implicated in X-chromosome

inactivation in female mammals. Inactivation of one of the

two female X-chromosomes occurs in mammals. In 1975 Riggs

was one of the first to hypothesize that X-chromosome

inactivation involved DNA methylation. This is an

interesting case of an epigenetic modification titrating

gene dosage.. One could imagine a theoretical case where

the female is programmed to extrude the extra X-chromosome.

This does not happen, and it is easy to speculate that

evolving the machinery to actively remove DNA might in the

long run pose more problems than it solves. While current

evidence supports a role for DNA methylation in X-

chromomsome inactivation, the details of how DNA

20

methylation participates in X-chromosome inactivation is

not completely understood (Csankovszki 1999).

Finally, the "host defense hypothesis" put forward by

Bestor states that DNA methylation functions primarily to

repress retroviral genes found throughout mammalian genomes

(Yoder, Walsh, and Bestor 1997). It is well established

that mammalian genomes contain huge regions of repeated DNA

sequences often of retroviral origin. These regions are

usually silent and cytosines in 5'-CpG-3' sites are

methylated. Empirical data show that when expression of

endogenous retroviral sequences occurs it is associated

with a lack of DNA methylation (Walsh et al 1998). Thus, 5-

methylcytosine may have a function in preventing the

expression of both exogenous and endogenous retroviral

sequences.

In conclusion, the base 5-methylcytosine, the only

endogenous alteration of the four bases that comprise DNA,

functions in mammalian development, cell differentiation,

gene activity, X-chromosome inactivation in mammalian

females, and may be important in silencing retroviral

sequences. Germane to the present study, recent advances

link abnormal levels and patterns of 5-methylcytosine to

human cancer (Holliday 1996).

21

Dysragula^on of S-aa-thylcyteaxn* In human eancar Involves

'the Inac^va'fci.on of sp«cl£lc ganas

There are two direct pieces of evidence that 5-

methylcytosine is dysregulated in human cancer: (1) total

5-methylcytosine content in cancer cells is decreased when

compared to normal cells, and (2) regional 5' CpG islands

in cancer cells show increases in methylation levels

(Holliday 1996).

Holliday first postulated in 197 9 that DNA methylation

may be involved in cancer (Holliday 197 9). His argument

stemmed largely from the failure of mutational data to

account for experimental observations of the frequency of

mouse cell transformation into cancer. The proposition

gained support with findings that global DNA methylation

levels were decreased in human cancer when compared to

normal controls. The study of Feinberg and Ehrlich in 1988

showed a decrease in total 5-methylcytosine in colon cancer

when compared to normal controls. It is speculated that

the vast regions of DNA not associated with expressed genes

and containing infrequent 5'-CpG-3' sites are normally

methylated, but in human cancer these cytosine become

demethylated. This might explain the global decrease in

22

DNA methylation observed in human cancer, concurrent to

regional increases in methylation discussed next.

A growing list of human genes that contain 5' CpG

islands have been shown to be inactivated by DNA

methylation in human cancer. Retinoblastoma (pRb) was one

of the first genes where inactivation by DNA methylation

was found to occur in cancer (Ohtani-Fujita et al 1993).

Since pRb is a classic tumor suppressor gene, the idea

emerged that any tumor suppressor that contains a 5' CpG

island may be subject to inactivation by DNA methylation

{Knudsen 1971, Baylin et al 1991). This is an area of

active research and the list of genes that are

hypermethylated in human cancer is still increasing. There

are examples of genes that are inactivated by

hypermethylation in human cancer and alter (1) response to

chemotherapeutics (MGMT), (2) tumor metastasis (E-

cadherin), and (3) cell growth (BRCAl, pl5, pl6, and p73)

(Watts et al 1997, Graff et al 1998, Herman 1999) . In

summary, regional increases in DNA methylation in 5' CpG

islands occur in human cancer in a variety of genes and is

associated with transcriptional silencing of the

corresponding gene.

23

In addition to the absolute changes in 5-

methylcytosine patterns and levels in human cancer, DNA

methylation is also implicated in mutation rates. It is

estimated that one-third of all the observed mutations in

human cancer occur at CpG sites (Denissenko 1997). This

finding links epigenetics to genetics and illustrates the

importance of further research to understand the complete

role of DNA methylation in human cancer. In conclusion, 5-

methylcytosine is definitively dysregulated in human cancer

and these changes influence both the transcriptional

activity of specific genes and the overall mutation rate in

cancer cells.

Loss of daoxycytidln* kinase (dCR) Is io^lxcated In drug

resistance and dCK xs a candidate for inactivetlon by DMA

methylation

Deoxycytidine kinase (dCK) is a gene involved in the

pyrimidine nucleotide salvage pathway. dCK is the rate-

limiting step in the activation of the prodrug cytosine

arabinoside (ara-C), which is used to treat acute myeloid

leukemia (AML). Retroviral introduction of dCK into ara-C-

resistant cells resulted in a ara-C-sensitive phenotype

(Manome et al 1996). While the loss of dCK in AML may

24

represent a mechanism of drug resistance, deletions or

mutations of dCK are infrequent in AML (Flasshove et al

1994) . Two provocative studies, one by Kong et al in 1991

and the other by Antonsson et al in 1987 sugg'ested that 5-

azacytidine, a demethylating agent, reversed drug

resistance in a dCK negative cell line by reactivation of

dCK. These two observations, coupled with the presence of

a 5' CpG island that regulates dCK gene expression, make

dCK a candidate gene for inactivation by DNA

hypermethylation (Chen et al 1995).

Pofcantial rol* of pl5 and pl6 m.m ^uBor si^prassors

The major proteins that regulate eukaryotic cell

cycles have recently been discovered and characterized. It

is beyond the scope of this document to review this area of

research, however, a brief description of one growth

regulatory pathway will be given. Kinases that depend on

the presence of cyclins, referred to as cyclin-dependent

kinases, or cdks, gate the cell cycle. A positive

association has been found between the kinase activity of

cdks and cell cycle progression. How these cdks are

regulated became the focus of gene discovery for much of

25

the 1990s, ultimately linking them to the tumor suppressor

gene retinoblastoma (pEUj) (Weinberg 1995).

pl6 was discovered by Serrano et al in 1993 using a

two-hybrid screen with cdlc4 as the bait. When pl6 bound

cdk4 or cdk6 it was shown to inhibit cdk4/6 kinase

activity. Subsequent to pl6's discovery, pl5 was

discovered by Hannon et al and Jen et al in 1994. pl5 and

pl6 lie adjacent to each other along chromosome 9p21. This

region of DNA produces three potential tumor suppressor

genes, pl6/pl9ARF, where pl9ARF is generated by the use of

a different exon 1 but the same exon 2 and 3 as pl6 (pl9

uses a different reading frame than pl6, hence pl9ARF =

Alternative Reading Frame), and pl5. The pl9ARF gene

product interacts in the p53 tumor suppression pathway by

binding to MDM2. Figure 1 illustrates the genomic

organization of pl5, pl6, and pl9ARF.

pl5 and pl6 share >80% protein homology and both bind

to and inhibit cyclin-dependent kinases 4 and 6 (cdk4/6).

pl5 and pl6 are 2 of the 4 members of the INK4 family

(INhibitor of cyclin-dependent Kinase ±) that also includes

pl8 and pl9. The protein homology between pl5 and pl6 is

shown in figure 2. In addition to the INK4 family, the

CIP/KIP family contains p21, p27, and p57 and each gene

26

functions to inhibit cdk2 paired with a specfic cyclin

(whereas the INK4 family only inhibits cdk4/6, bound to D-

type cyclins 1,2, or 3). The pathway in which pl5 and pl6

are thought to function is depicted in figure 3.

Ultimately it is believed that pl5 and pl6 prevent the

phosphorylation of pRb which in turn prevents the release

of the transcription factor E2F, and E2F dependent

transcription of S-phase genes.

pl5 and pl6 were originally implicated in human cancer

because both lie on a stretch of chromosome 9p21 frequently

deleted in human cancer (Kamb et al 1994). Further, pl6

mutations were shown to occur in familial melanoma

(Hussussian et al 1994) . While deletion of pl5 occurs in

human cancer, it is only rarely a pl5 exclusive deletion

that does not also delete pl6/pl9ARF, and mutation of pl5

has not been observed in any human cancer. Nevertheless,

pl5 and pl6 are both subject to inactivation by

hypermethylation in hematological malignancies.

Specifically, Herman et al 1997 used Southern blots to show

that pl5 but not pl6 is frequently hypermethylated in AML.

Thus, pl5 may have a role in tumor supression in AML

despite an unaltered pl6 gene.

Figure 1. A schematic map of the genomic structure of the region of DNA on human chromosome 9p21 that encodes pl5, pi6, and pl9ARF. The green boxes depict exons 1 and 2 of pl5, the blue boxes depict exons la, 2, and 3 of pl6, and the red box depicts exons ip that comprises pl9ARF along with the blue boxes of exons 2 and 3. The approximate locations of the the three 5' CpG islands is shown in the yellow boxes.

28

NHAR

pl5

pl6 IDAAEGPSDIPD*

Figure 2. The protein homology between pl5 and pl6 is shown as the gray shaded regions. The red shading indicates amino acids in pl6 that bind to cdk6 and are mutated in human cancer, resulting in a loss of pl6 function. Surprisingly, the red shaded amino acids of pl5 are not mutated in human cancer.

p15/p16

6

29

Figure 3. The pathway that pl5 and pl6 participate in is shown in this cartoon. Both pl5 and pl6 bind to cdk4 and cdk6 and inhibit the kinase activity of cdk4 and cdk6. In the absence of pl5/pl6 unregulated phosphorylation of retinoblastoma (pRb) promotes entry of the cell into S-phase.

30

StateBMn^ of puxpoum ot pr«s«nt steditts

The present study was designed to define target genes

that are hypermethylated in AML (figure 4, next page, shows

a summary). We hypothesized that hypermethylation of 5'

CpG islands is associated with transcriptional silencing of

the corresponding gene and participates in either the

emergence of drug resistance or the conversion of normal

cells to cancer cells.

Since dCK was known to have reduced activity in

cytosine-arabinoside (ara-C)-resistant leukemia cell lines,

and no deletion or mutation accounts for the loss of dCK

activity, dCK represents a mechanism of drug resistance and

is a candidate gene for inactivation by hypermethylation.

It was known from Southern blot data that pl5 but not

pl6 is methylated in AML. Both pl5 and pl6 are thought to

be tumor suppressor genes, genes capable of preventing the

conversion of normal cells to cancer cells. pl5 and pl6

are adjacent to each other, have >80% amino acid identity,

and yet only pl5 is hypermethylated in AML. In table 1,

page 33, the cell line models studied are summarized. We

used this situation to describe the methylation of pl5 and

try to understand why such a situation arises in AML.

31

Identification of Candidate Genes that are hypermethyiated in AML

dCK methylated dCK not methylated (Chapter 3)

p15 or pi 6 methylated, p15 methylated (Chapter 4)

pi 5 or pi 6 not methylated

Introduction off pi 5 or pi 6 into Jurkat (Chapter 5)

Figure 4. An overview of the experiments presented in this dissertation. Initially we determined the methylation status of deoxycytidine kinase (dCK) in cell line models and AML patients, (Chapter 3). Once a lack of dCK methylation was demonstrated, the focus shifted to pl5 and pl6 methylation methylation analysis (Chapter 4) . When pl5 methylation of AML cell lines and patients samples in the absence of pl6 alterations was detected, the final Chapter focused on the functional contribution of each (Chapter 5).

32

KG-1 AML No detectable pl5, but pl6 detectable

KG-la AML No detectable pl5, but pl6 detectable

HL60 AML pl5 detectable

U937 AML pl5 detectable

HaCaT Keratinocyte Positive control for pl5 detection

RHEK-1 Keratinocyte Positive control for pl6 detection

Jurkat T-ALL Negative control for both pl5 and pl6 detection

Melanoma UACC 612

Melanoma P15 detectable, but no detectable pl6

Table 1. A summary of the names and types of the cell lines used to determine pl5 and pl6 mRNA levels by RT-PCR and protein levels by immunoblots.

33

CHAPTSR 2 - MXTXRXALS AND METHODS

Call cultux*

HL60-sensitive and HL60-daunorubicin resistant cells

were a gift from Dr. K. N. Bhalla at Emory University, and

K562-sensitive and K562-daunorubicin resistant were a gift

from Dr. S. Grant at Virginia University (Bhalla et al

1984, Grant et al 1995). Jurkat, U937, KG-1, and KG-la

were obtained from ATCC. HaCaT was established by Dr.

Fusenig and we obtained it from Dr. Bowden's lab at the

Arizona Cancer Center (BouJcamp et al 1998). HL60/S,

HL60/R, K562/S, K562/S, U937, and Jurkat were cultured in

RPMI 1640 supplemented with 5% (Jurkat) or 10% (HL60/S,

HL60/R, K562/S, K562/S, and U937) FBS. KG-1 and KG-la were

cultured in IMEM supplemented with 20% FBS. Melanoma

UACC612 was established from a patient with melanoma at the

Arizona Cancer Center core facility. RHEK-1 was obtained

from Dr. Johng S. Rhim (Rhim et al 1985) . HaCaT and RHEK-1

were cultured in DMEM supplemented with 10% FBS All

cultures were maintained in penicillin (100 U/ml), and

glutamine (1% vol/vol) (JRH Biosciences, Lenexa, KS) and

incubated in 95% air-5% C02 atmosphere at 37° C.

34

Normal c«lls and pa^ant mmmplmm obtaxnad for usa in tbxa

study

Peripheral blood or bone marrow specimens were

obtained from healthy allogeneic bone marrow donors and 8

AML patients after informed consent (see table 1 for more

information). From these samples low density mononuclear

cell fractions were isolated by double Ficoll-Hypaque

density centrifugation (Pharmacia, Uppsala, Sweden) or by

the Vacutainer CPT cell preparation system in the case of

the normal PBLs (Becton Dickinson, Franklin Lakes, NJ).

Isolation of AML patient specimens was performed by Dr.

Alan List's lab at the Arizona Cancer Center and yielded

>85% blasts as determined by cytologic examination.

DHA xsola1:i.on and Southam blot analysxs

DNA was isolated with a QIAamp blood kit isolation kit

according to the manufacturer's protocol. The DNA was cut

with appropriate restriction enzymes (SU/fXL) at 37° C. The

digested DNA was phenol/chloroform purified, precipitated

with 0.1 volume 3M sodium acetate and 2.5 volumes 95%

ethanol, and pelleted by 30 minute spin on a microfuge at

maximum speed at 4° C. The DNA was resuspended and

quantitated spectrophotometrically by OD at 260 nm. 10 (ig

of cut DNA was size separated by gel electrophoresis on a

1% agarose gel. The DNA was de-purinated with 0.2 M HCl

35

for 15 minutes, denatured with a solution of 0.5 M NaOH and

1.5 M NaCl for 30 minutes, and neutralized with a pH 7.4

solution of 0.5 M NaOH, 55 mM Trizma-HCl for 30 minutes.

The DNA was then capillary transferred in lOX SSC (3M NaCl,

0.3M sodium citrate) from the gel to a 0.45 nm Nytran

membrane overnight. The membrane and DNA were crosslinked

by UV light, sealed in a membrane with ~5 mL pre-

hybridization solution (50% formamide, 5X SSC, IX

Denhardt's solution [lOOX Denhardt's solution is: 20 mg/mL

Ficoll 400, 20 mg/mL polyvinylpyrrolidone, and 20 mg/mL

bovine serum albumin fraction five], 1% sodium dodecyl

sulfate, 10% dextran sulfate, and 250 ng/mL salmon sperm

DNA) followed by incubation overnight at 42° C with

shaking. radio-labeled DNA probe of the dCK cDNA was

then generated by random primer labeling, briefly -25 ng

template DNA was labeled using the Gibco BRL Radprime kit

with 5 |iCu of a-dCT^^P. The labeled probe was boiled for 5

minutes and added to the pre-hybridization solution and

allowed to hybridize overnight at 42° C. The membrane was

washed at room temperature in 2X SSC, 0.5% SDS for 30

minutes, then 2 washes in 0.IX SSC, 0.5% SDS at 55° C were

performed. The membrane was exposed to x-ray film with

intensifying screens at -80° C.

36

RMA isolation and Northttxn blot analysis

RNA was isolated with Qiagen Rneasy kit according to

the manufacturer's protocol. The isolated RNA was then

quantitated with a spectrophotometer by absorbance at 260

nm. 20 (ig of RNA in ~11 |i.L of H2O was denatured with 4 (iL

lOX MOPS buffer, 7 |iL 37% formaldehyde solution, and 16 }iL

de-ionized formamide and heated at 55° C for 15 minutes.

2 (iL of RNA loading buffer (50% glycerol, 1 mM EDTA, 0.25%

bromophenol blue) were added, and the RNA then loaded onto

a denaturing formaldehyde/agarose gel (IX MOPS buffer, 18%

vol/vol 37% formaldehyde, 1% agarose). The gel running

buffer was IX MOPS with ethidium bromide added to visualize

the RNA. After electrophoretic separation at 60 volts, the

formaldehyde was leached out of the gel by one wash in IX

MOPS for 15 minutes, followed by two 15 minute washes in

DEPC-treated H2O. RNA was capillary transferred to a 0.45

|im Nytran membrane as described in Southern blots above.

The membrane and RNA were UV crosslinked, and then the pre-

hybridization and hybridization were performed as described

for Southern blots above.

Revarsa-transeriptas* polyaarasa chain raaction (RT-PCR)

Total cellular RNA was isolated using the RNeasy minikit

(Qiagen) and quantitated using a spectrophotometer

measurement at 260 nm. For pl5 and pl6 33 cycles were

37

used, and for histone 3.3 25 cycles were used. The primers

used for pl5, pl6, and histone 3.3 (H3.3): were

dCK 5' (5'-CATTTGTGAATATCCTTAAAC-3'),

dCK 3' (5'-ATAAATGATTCCATCCAATTCA-3') ,

p15 5'2 {5'-TGGGGGCGGCAGCGATGAG-3'),

pl5 3' (5'-TGGGTAAGAAAATAAAGTCGTTG-3') ,

pl6 5' (5'-AGCCTTCGGCTGACTGGCTG G -3'),

pl6 3' (5'-CTGCCCATCATCATGACCTGGA-3'),

H 3 . 3 5' (5'-CCACTGAACTTCTGATTCGC-3'),

H3.3 3' (5'-GCGTGCTAGCTGGATGTCTT-3').

These reactions were carried as follows: 2 pg of total

cellular RNA was reverse transcribed by incubating a 20 pi

reaction mixture containing IX PGR buffer (10 mM Tris [pH

8.3], 50 mM KCl, 6 mM MgCl2), 2 mM each dATP, dCTP, dGTP,

and dTTP, 200 pmol random hexamer, 20 U Rnasin (Roche), and

200 U Superscript II reverse transcriptase (Gibco BRL) at

42*^0 for 60 min. The reaction was stopped by incubation at

99^C for 10 min. Analysis of pl5 and pl6 expression was

performed by adding 10 pi of the RT reaction to 40 ul of

amplification reaction mix (IX PGR buffer, and 1.25 U of

Tag DNA polymerase) followed by incubation at 98*^0 for 5

min; 33 cycles of 98^0 for 30 s, 56^C for 30 s, 12^C for 1

min; and a final extension at 12^C for 5 min followed by a

quick chill to 4®C. Analysis of Histone 3.3 was performed

by adding 1 pi of the RT reaction to 4 9 pi of amplification

38

reaction mix (IX PGR buffer, and 1.25 U of Taq DNA

polymerase) followed by incubation at 94^C for 5 min; 25

cycles of 94^C for 1 min, 56^C for 30 s, 72®C for 1 min;

and a final extension at 7 2^C for 5 min followed by a quick

chill to 4^C. For analysis, 20% of the respective PGR

products were separated on 2% agarose gel, visualized by

ethidium bromide staining with the Eagle Eye II Still Video

System (Stratagene, La Jolla, Ga.). In the case of semi-

qunatitative RT-PGR for dGK and His 3.3, the desired cycles

were performed and 20% visualized and staining intenisty

quantitated by ethidium bromide staining with the Eagle Eye

II Still Video System.

Genera^on o£ pl5 aRHIi by in vlteo fcranscripti.on for umm mm

a posx'ti.v'* control

The full length coding sequence of pl5 was obtained

from normal human bone marrow by 35 cycles of RT-PCR as

described above with primers pl5 3' and pl5 5'1, (5'-

CAGGAAAAGGCGGGAGGTAAGGA-3'), and ligated into pGEM T-easy.

The T7 primer generated sense pl5 RNA using the Boehringer

Mannheim in vitro transcription kit according to the

manufacturers protocol. The resulting pl5 RNA was then

used to establish the RT-PGR protocol, and in subsequent

RT-PGR experiments the pl5 cDNA was used as a positive

control.

39

Prot«xn xsola^on and lUmutmxn blo^

Total protein was obtained by treating cells with

lysis buffer (50 mM Tris-HCl, 250 mM NaCl, 0.5% NP-40, 50

mM NaF) containing protease inhibitors (1 mM PMSF, 20 Dg/Dl

N-TPCK, 20 mg/ml STI, 10 mg/ml leupeptin, 0.066 TI units/ml

aprotinin) for 60 minutes on ice. Lysates were spun for 5

minutes at 13,000 rpm to remove debris. Supernatants were

taken for protein quantitation using BSA standards (Pierce,

Rockford, IL). In the case of TGF-B treated cultures,

exponentially growing cultures were treated with 2ng/mL

TGF-Bl for 24 hours (Sigma, St. Louis, MO). After

quantitation, 0.25 mg of protein (except HaCaT -/+ TGF-I5

where 0.1 rag was used) from each cell line was denatured in

SDS-PAGE sample buffer (1 ml glycerol, 0.5 ml 2-

mercaptoethanol, 3.0 ml 10% SDS, 1.25 ml 1.0 M Tris-HCl pH

6.7, 1 mg bromophenol blue) and the samples were subjected

to SDS-PAGE on a 15% pre-cast mini gel (Bio Rad, Hercules,

CA). The resolved proteins were transferred onto a

Immobilon-P membrane by electrophoretic transfer at 60

Volts for 4 hours at 4° C (Millipore, Bedford, MA). The

nonspecific sites were blocked by incubation in 5% nonfat

dry milk in Tris-buffered saline and 0.05% Tween 20 (TEST)

for 1 hour at room temperature. The membrane was then

incubated with pl5 antibody (sc-612 Santa Cruz, CA) 1:50

40

dilution in TBST or pl6 antibody (sc-468 Santa Cruz, CA)

1:100 dilution for 1 hour at room temperature. The

membrane was washed with TBST and incubated with

horseradish-peroxidase-conjugated immunoglobulin G

secondary antibody (Jackson Immunoresearch, West Grove, PA)

for 1 hour at room temperature. Following 3 quick rinses

and 3 15 minute washes with ~10 mL TBST all at room

temperature, detection by chemiluminescence was performed

with the Renaissance Kit (DuPont NEN, Boston, MA) and

exposed to film (XAR-5, Eastman Kodak Co., Rochester, NY).

6«nerat:xon of pl5 rscfbi nanfc protaxn for us* as a posx^va

control

The pl5 cDNA was obtained from normal human bone

marrow by RT-PCR as described above. The pl5 cDNA was

subcloned with two EcoRI sites into the pMAL-c2 vector (New

England Biolabs, Beverly, MA). The resulting vector

pl5MAL-c2 was sequenced to confirm its protein coding

sequence and orientation. pl5MAL-c2 was transfected into

competent E. coll (Invitrogen). A log-phase culture was

used to column purify pl5 and the resulting isolate was cut

with factor Xa to yield pl5 protein.

41

BxauXfxt* ••qu«nexn9 of dCK, pl5, and pl6

DNA was isolated from the cell lines, normal tissue

specimens, and AML patient samples (as previously

described) using the QIAamp blood kit (Qiagen, Santa

Clarita, CA), and quantitated spectrophotometrically at 260

nm. Sodium bisulfite conversion followed the protocol of

Clark et al 1994. Briefly, DNA was denatured in 0.3 M NaOH,

reacted with 3.6 M sodium bisulfite (pH 5.0) at 55° C for

14 hours, desalted with the Wizard Prep kit (Promega,

Madison, WI), desulfonated with 0.3 M NaOH, and ethanol

precipitated. The resulting bisulfite-modified DNA was

then amplified using nested PGR. The first reaction used

-500 ng of DNA with IX PGR buffer, 200 uM dNTPs, 50 pmol of

either Al & A2 (1st round) or B1 & 32 (2nd round), and 2.5

U Taq polymerase (Roche, Indianapolis, IN). The 2nd round

of PGR used 1-10% of the 1st round reaction under identical

conditions. The following bisulfite specific primer sets

were used,

dCK 5' : dCKUl (5'-TTTGTTTATTTTTAATAGGTTTATTAGAG-3' )

dGKDl (5•-AATCCCGTGAAAACTAACTAAAAAAAA-3')

dGKU2 (5'-GGTTTTTGGGGTTTATTTTTTTTTTT-3')

dGKD2 (5'-AAATAAGGATTCGTTAATCTTATA-3')

pl5 5' : P155U1 (5'-TTGTATGATAGGTGTAGAGTTG-3')

P155U2 (5'-GTATTGTTTGGGGATGAATTTAA -3')

P155D1 (5'-GTGTAACAAAATAAAAAAGGAAG-3')

42

P155D2 (5'-AAATCCTCACTACCCCICCTCIC-3' )

pl5 3^: P153U1 (5'-GGTTTTTTGGTTTAGTTGAAAA-3')

P153U2 (5'-AACITAAACTCCTATACAAATCTACAT-3')

P153D1 {5'-TGTIGGTTGGTTTTTTATTTTGTTAGA-3')

P15 3 D2 ( 5 ' -AAACCCTAAAACCCCAACTACCTAAAT - 3 ' )

pl6 5": P165U1 (5'- TTAGTIGTATAGGTGATTTIGATTT -3')

P165U2 (5'-GGTTGAGGGGGTAGGGGGATAT-3')

P165D1 (5'-CCCCACCCTCTAATAACCAAC-3')

P165D2 (5'-TACCCCTCTCCICAACCICCAAAC-3' )

pl6 3' : P163U1 (5 *-GGTTGGTTGGTTATTAGAGGGTGG-3')

P163U2 ( 5 ' -TACAAACCCTCTACCCACCTAAAT-3 ' )

P163D1 (5'-GTTGGTTATTAGAGGGTGGGG-3')

P163D2 {5'-CTCCIACCITAACTATTCIATAC-3')

Amplifications were performed as follows: 95° C 1 min,

followed by 35 cycles of 92° C 1 min, ramp 1.0° C/sec to

56° C, 56° C 3 min, 0.3° C/sec to 72° C, 72° C 1 min, 0.5°

C/sec to 92° C. There was a final extension at 72° C 5 min

and a quick chill to 4° C. All PCRs were performed on a

DNA engine (MJ Research, Watertown, MA). The PCR products

were ligated into the vector pGEM T-easy (Promega) and

transfected into competent E. coli (Invitrogen, San Diego,

CA). Plasmid DNA was isolated from the resultant bacterial

colonies using a QIAprep Spin Plasmid Miniprep kit

(Qiagen), and positive recombinants were sequenced on an

ABI automated sequencer. The resulting sequences were

43

aligned to their respective sequences using AssembyLIGN

software. The number of methylated CpGs at a given site

was divided by the number of clones analyzed (n = 5-11,

except HL60 pl6 where n = 2) to yield a percent

methylation.

Transi«n^ transfttc^on wxth CAT gan* r«port«r cons^ructe

HaCaT cells were plated 24 hours prior to transfection

at ~50% confluency, and transfected with lipofectamine

(Gibco BRL). The wild-type pl5 promoter region was

amplified from normal bone marrow and three regions were

then subcloned into pCAT with Pst I sites after first

adding a Pst I site into the 5' primer and initial TA

cloning into pGEM T-easy. Four micrograms of each

construct were used per transfection and an SV40f3GAL

plasmid served as a control. Activity was detected 48

hours after transfection with CAT and BGAL ELISA assays

(Roche), and total protein was quantitated with BSA

standards (Pierce).

Selec^on of stabl* •xpr«ssion of pl5 and pl6 in coll linos

Jurkat Tet-Off cells and tetracycline inducible

expression system were purchased from Clontech. The pl5

cDNA was subcloned into the EcoRI site of the pTRE vector.

The resulting vector plSpTRE was sequenced. In addition.

44

the hygromycin resistance gene was subcloned from the

pTKHyg vector into the plSpTRE and pl6pTRE vectors with

Xhol sites. The resulting vector, plSpTREpHyg,

pl6pTREpHyg, or pTKHyg (as control for the effects of

hygrom.ycin resistance) were then used for transfections.

Transfection of 1 x 10^ Jurkat Tet-Off cells with 2 fig of

pTKHyg, plSpTREpHyg, or pl6pTREpHyg, and in the case of

double plasmid selection, 2 ̂ g of pTKHyg and 40 |ig plSpTRE

were performed on a Biorad gene pulser set to 250 mV and

960 (IF. The cells were cultured without selection for two

days after electroporation, then bulk selected with 400

(ig/mL hygromycin (Clontech) for 3 days, and finally clonal

populations were obtained by limiting dilution in 96-well

plates. The clonal populations were tested for pl5 or pl6

DNA and RNA presence by PGR or RT-PCR.

45

The individual clones were obtained from plates with

from 4-15 clones per 96-wells. Poisson statistics yield a

probability with the following mathematical argument.

Assuming 9.6 clones/96-well plate, 1 in 10, X = 0.1,

H = Xv, describes the total occurance, where V is the volume

of the well, in this case V = l, soM.= 0.1. Then the

probability, Pn, can be expressed as:

Pn = (i^e-^'/N!, where N = the number of cells that form a

colony, N = 1 for the desired clonal colonies, from this

the probabilities are: (1) no colony forms = 90.5%, (2) a

clonal colony forms = 9.05%, and (3) two cells initiate a

colony = 0.005%. Thus the average 96-well plate yielded 10

colonies which was a > 1000-fold more likely generated by

one cell than by two.

T6F-B, PIA, PIA/IonoHYcxn, eytesln* arablnosld* (ara-C) and

daunorubicin traafant of call cultuxaa

TGF-13, PMA, and lonomycin were all solubilized

according to the manufacturers recommendation (Sigma).

Cytosine arabinoside and daunorubicin were obtained from

the tumor cloning lab at the Arizona Cancer Center. The

46

desired doses were added directly to the cell cultures and

incubated at 37° C.

HTS assay for drug s«nsi.^vi.ty

The cells were counted and plated at 8,000 cells/well,

100 |J.l/well on day 1. The appropriate dose of drug was

delivered 24 hours later on day 2. At day 6 the MTS kit

(Promega) was used according to the manufacturer's protocol

and results were read by absorbance at 470mn.

FACS analysis of e«ll cycla by propidiuB lodxd* s^inxng,

FACS analysis of apoptosls by Annaxln V/PI staining, and

cell groirth In liquid cultura

Cells were washed with PBS, and resuspended in

Krishnan's buffer containing 50 ng/mL propidium iodide, 20

(ig/mL RNase, 0.3% NP-40. Annexin V (Boehringer Mannhiem)

and prodium iodide were added to washed cells according to

the manufacturer's protocol and were analyzed by FACS. The

core facility at the Arizona Cancer Center performed FACS

analysis on both samples. Growth in liquid culture was

performed by plating equal cell numbers in 6-well plates

and counting cells daily with a cytometer.

Mlcroarray axprasslon analysis

Probe Preparation: The human cDNA bacterial clones

used to fabricate the microarray came from Research

47

Genetics (Huntsville, AL). Referred to as gf200, the set

consists of 5,184 sequence-validated IMAGE consortium

bacterial clones, approximately 3,000 of these clones

represent known genes while the remainder are unknown ESTs.

cDNA targets were produced by PGR of the cDNA inserts

directly from bacterial cultures. In brief, individual

IMAGE clones were grown in 96-well plates at 37 °C for 6

hours. One microliter of the bacterial culture was added

to a PGR reaction and the cDNA inserts amplified in a 96-

well format using a PGR primer pair (Research Genetics)

designed to selectively amplify the cDNA inserts contained

within the IMAGE clones. Primers and unincorporated

nucleotides were removed from the PGR products using a 96-

well PGR clean up kit from Qiagen. PGR amplification and

clean up were verified by agarose gel electrophoresis, and

PGR product yield was determined using a PicoGreen-based

fluorescence assay (Molecular Probes, Eugene, OR) in a 96-

well format. After quantitation the purified PGR products

were dried and re-suspended at 300 ng/)jl in 2X SSG for

printing onto slides.

Microarray Fabrication: The purified, PGR-amplified,

cDNAs were printed onto chemically-activated glass slides

48

(CEL industries, Houston, TX) using 4 quill-type pins

(Telechem International, San Jose, CA) mounted onto an

OmniGrid robot (GeneMachines, Menlo Park, CA). In addition

to the 5,184 IMAGE clones, a set of housekeeping genes

{Research Genetics), a set of Mesembzyanthemum

crystallinum (ice Plant) genes, and Cy3 or Cy5 (Amersham)

labeled oligonucleotides were placed strategically to aid

in data normalization, measuring non-specific

hybridization, and locating the corners of the array.

Finally, a set of 103 IMAGE clones representing known genes

that were not included in gf200 were purchased from

Research Genetics and included in the microarray.

Following printing, the slides were placed in a humidity

chamber overnight in the dark to re-hydrate the spots of

cDNA probes. The next day the slides were washed one minute

in 0.1 % sodium dodecyl sulfate (SDS) and one minute in

double distilled water at room temperature. Slides were

then submerged in a 75% v/v water/ethanol solution into

which 0.6 g sodium cyanoborohydride had been dissolved for

five minutes at room temperature followed by four washes in

double distilled water for two minutes each. Slides were

then spun dry at 500g and stored in the dark at room

temperature until use.

49

Target Preparation: poly A+ RNA was isolated from ~50

X 10^ cells using the midi/maxi oligotex direct kit

according to the manufacturer's protocol (Qiagen).

Fluorescent first strand cDNA was made from 4 ng of poly A+

RNA in the presence of 50 HM Cy5-dCTP (green) or Cy3-dCTP

(red) in a 25 |J.l volume containing the following: 500 ng

oligo (12-18) dT, 1 X Superscript Buffer, 400 U Superscript

II, 3.3 U RNAse inhibitor (all from Gibco BRL), 400 |iM each

of dGTP, dATP, dTTP, 100 HM dCTP, and 10 mM dithiothreitol.

All reagents except the Superscript II were mixed on ice,

placed at 65 °C for five minutes, and 25 °C for 5 minutes at

which point the Superscript II was added and the mixture

heated to 42 °C for two hours. The mRNA was then degraded

by heating the reaction for five minutes at 95 °C, adding

6.25 fJ-l of 1 M NaOH, and a final 10 minutes incubation at 37

°C. Labeled cDNA from two reactions (Cy3 or Cy5 labeled)

was purified on a microcon-50 column using four buffer

exchanges (the first three were water, the final exchange

was 10 mM Tris-HCl, pH 8.5), eluted from the column,

lyophylized to dryness, and re-suspended in 10 (4.1

hybridization buffer (2 X SSC, 0.1% SDS, 100 ng/^l Cotl DNA,

50

100 ng/^l oligo dA), denatured by boiling for 2.5 minutes,

and added a denatured (boil slide 2 minutes, plunge into

room temperature ethanol, and spin dry at 500g) microarray.

A cover slip (22 x 22 mm) was used to spread the target

evenly over the probes and the array was placed in a

hybridization chamber (Telechem International) at 62 "C for

18 hours. Following hybridization, slides were washed by

placing them into 50 mL conical tubes containing 2 x SSC,

0.1% SDS for five minutes, 0.06 x SSC, 0.1% SDS for five

minutes, and 0.06 x SSC for two minutes all at room

temperature. Quantitative fluorescent emissions were

collected using a Scan Array 3000 microarray reader

(General Scanning Inc.) and quantitated using the Imagene

software (version 2.0, Biodiscovery Inc.). Three

independent pl5 or pl6 positive Jurkat clones were arrayed

against the pl5 and pl6 negative parent cell line and

cumulative results were used to identify differentially

expressed genes.

51

CHAPTKR 3 - DSTBRMZHATZOT OF S-MBTHTLCTTOSZIIE

INFLUENCE ON dCR EXPRESSION

Dnig-sttnsx^v* and -rMlstanfc modml c«lX IxnM

The hypothesis of our initial efforts (see figure 4

for a complete overview of the research presented in this

dissertation) was that DNA hypermethylation is associated

with decreased dCK expression and this loss of dCK

expression participates in the drug resistant phenotype.

In an effort to better understand the role of dCK

expression levels in the emergence of resistance to

cytosine arabinoside (ara-C), a drug used to treat acute

myeloid leukemia (AML), the paired ara-C-sensitive (/S) and

ara-C-resistant (/R) cell lines, K562/S and K562/R, and

HL60/S and HL60/R were obtained. K562/R was reported by

Grant et al (1995) to contain 70% less dCK activity than

the sensitive parent cell line, and Bhalla et al reported

(1984) that HL60/R was deficient in dCK activity. These

reports showed that loss of dCK activity is central to the

araC-resistant phenotype. Further evidence in the

literature suggests that exposure to 5-azacytidine, an

inhibitor of DNA methylation, re-activates dCK in drug-

resistant cells, supporting the hypothesis that DNA

52

methylation mediates the loss of dCK expression in drug-

resistant leukemia cells (Kong et al 1991, Antonsson et al

1987) .

dCK gene atxuctnxm and •a^pr^ssion in aodal c^ll lin«s

In order to determine if an association between dCK

and ara-C-resistance existed we first performed a Southern

blot using the complete dCK cDNA as a probe. It might be

the case that one or both alleles containing dCK are

deleted or rearranged in the ara-C-resistant cell lines,

and this would explain the loss of dCK activity independent

of DNA methylation changes. The Southern blot, shown in

figure 5, did not reveal any gross changes in dCK gene

structure. The dCK cDNA probe showed similar intensity

and banding patterns in normal human peripheral blood

lymphocytes (PBL) and in the paired ara-C-resistant model

cell lines, K562/S and K562/R, and HL60/S and HL60/R.

These results indicate that the reported loss of dCK

activity is not mediated by deletion or rearrangement of

dCK at the DNA level.

53

9.42Kb

M 1 2 3 4 5 6 7 8 9 1 0

m m

2.03Kb

0.56Kb

Figure 5. Southern blot using the dCK cDNA as a probe with EcoRl digested genomic DNA. Genomic DNA was cut with EcoRl, recovered, and 10 (ig/lane was size separated by gel electrophoresis on a 1% agarose gel. The lane designated 'M' = Hindlll digested lambda DNA and served as a marker, the sizes in kilobases (Kb) are indicated on the left with arrows. Lanes 1-5 correspond to PBL, K562/S, K562/R, HL60/S, and HL60/R of the ethidium bromide stained agarose gel prior to transfer to a nytran membrane. Lanes 6-10 correspond to PBL, K562/S, K562/R, HL60/S, and HL60/R of the nytran membrane blot probed with the ^^P-labeled dCK cDNA.

54

The mRNA levels of dCK were determined in the model

cell lines by two techniques. Northern blot and semi­

quantitative RT-PCR. A representative Northern blot is

shown in figure 6 (n of 3 independent blots were performed

for dCK and GAPDH). Expression levels derived from the

Northern assay were normalized to GAPDH expression levels.

Northern analysis revealed an approximate 50% decrease in

dCK mRNA content in K562/R and HL60/R when compared to

K562/S and HL60/S respectively. For semi-quantitative RT-

PCR, various cycle numbers for both dCK and Histone 3.3

were performed to determine the linear range of PGR

amplification, shown in figure 7. The results were

quantitated by ethidium bromide staining of a 2% agarose

gel and detection of staining intensity using the

Stratagene Eagle-eye, shown in figure 8. The results

obtained with semi-quantitative RT-PCR also indicated an

approximate 50% decrease in dCK mRNA in both the K562 and

HL60 ara-C-resistant cells.

55

Figure 6. Northern blot for dCK. 20 \iq of total RNA was size separated by gel electrophoresis on a 1% agarose/ formaldehyde gel, ethidium bromide staining prior to transfer of the gel to a nytran membrane is shown on the right. After the gel was transferred to a nytran membrane, the membrane was probed with the ^^P-labeled dCK cDNA and then GAPDH. Lanes 1 -4 correspond to K562/S, K562/R, HL60/S, and HL60/R. Lanes 5-8 correspond to K562/S, K562/R, HL60/S, and HL60/R, and show the ethidium bromide staining of the 28S and IBS ribosomal RNA bands prior to transfer of the gel to a nytran membrane.

56

Btixidium bromide staxnxng intensity

le+5

le+4 16 18 20 22 24 26

17-25 cycles o£ RT-PCR for Hxstone 3.3

Ethidixwi bromi dn staining intensity

le+4 24 26 28 30

23-31 cycles o£ RT-PCR for dCK

Figure 7. HL60/R total RNA, 100 ng/reaction for histone 3.3 and 500 ng/reaction for dCK was used to determine the linear range of RT-PCR amplification. Shown on the y-axis is arbitrary ethidium bromide staining intensity, and on the x-axis is the number of PGR cycles. The blue arrows indicate the cycle numbers within the linear range chosen for semi-quantitative RT-PCR of dCK, 25 cycles, and Histone 3.3, 20 cycles.

57

M 1 2 3 4 5 6 7 8 9 1 0

Figure 8. Semi-quantitative RT-PCR for dCK. RT-PCR was performed for dCK (500 ng total RNA for 25 cycles/xeaction) and histone 3.3 (100 ng total RNA for 20 cycles/reaction), and then ran on a 2% agarose gel. The ethidium bromide staining intensity was determined with the Stratagene Eagle-eye software. Lanes: M = 100 base pair ladder, 1 = mock dCK, no RNA added, 2-5 = K562/S, K562/R, HL60ys, and HL60/R, 6 = mock Histone 3.3, no RNA added, and 7-10 = K562/S, K562/R, HL60/S, and HL60/R.

S8

DNA mathylatlon napping o£ tha 5' dCR Cp6 Island in nodal

cell Unas, noxnal human parxpharal blood lyaphoeytea

(PBL) , and acuta nyaloxd laukanxa (AML) patxants

The 5' maximal promoter region of the dCK gene is a

CpG island (Chen et al 1995). For this reason, we

hypothesized that dCK may be subject to DNA methylation

inactivation. To test this, we performed sodium bisulfite

sequencing of 49 5'-CG-3' sites in the dCK CpG island of

PBL, the paired ara-C-sensitive and ara-C-resistant human

leukemic cell lines K562/S, K562/R, HL60/S, and HL60/R, as

well as eight AML patients obtained from patients

refractory to ara-C-based chemotherapeutic regimens, see

table 2. The biochemistry underlying the sodium bisulfite

modification that allows for a positive display of those

cytosines that are methylated is shown in figure 9. The

region analyzed covered the maximal promoter region of dCK

from -228 to +143 relative to the transcription start site

(Chen et al 1995). In the paired ara-C-sensitive and ara-

C-resistant cell lines, K562/S, K562/R, HL60/S, and HL60/R,

no increase in cytosine methylation of the dCK CpG island

was seen. In fact, no cytosine methylation of the 5' dCK

CpG island was detected in the ara-C-resistant cells, see

figure 10, In normal PBL, all 49 CpG sites within the 5'

59

dCK CpG island were unmethylated. Similar to normal PBL

and the leukemia cell lines studied, 5 of 8 AML specimens

were completely unmethylated, and 3 of 8 had only 20%

methylation of one CpG site, see figure 11. In addition to

the results presented here, two independent investigations

have also failed to find methylation of dCK in drug-

resistant cell lines (Leegwater et al 1998, Fryxell et al

1999). In summary, the results we obtained indicate that

dCK mRNA is decreased in araC-resistant leukemia cell

lines, however the dCK 5' CpG island was unmethylated in

normal PBL, araC-sensitive and araC-resistant cell lines,

and ara-C-resistant AML patients. Thus, the mechanism for

the observed decrease in dCK expression is idiopathic.

The results presented here clearly demonstrate that

aberrant DNA methylation is not the only mechanism

responsible for decreases in gene expression that act as a

mechanism of drug resistance. The idiopathic decrease in

dCK gene expression is worth trying to understand, however

we decided to focus our effort on understanding aberrant

DNA methylation. For this reason, we chose to switch our

research efforts to pl5 and pl6, two tumor suppressor

genes, that had already been shown to be aberrantly

methylated in human cancer.

60

NH NH

O N ̂ SO," o-̂ N so

cvn,s.„.(0^ /""/ "

NH

CH

H H

5-Methylcytoslne Uracil

Figure 9. The biochemistry underlying the sodium bisulfite modification to define the methylation status of all cytosines within a PGR amplified region of DNA. Only unmethylated cytosines are converted to uracil which in the course of PGR is read as a T (T = 5-methyluracil), this results in a transition from G to T. Thus, only the cytosines methylated in the original DNA sample are retained after PGR. The PGR products are cloned and multiple sequences analyzed to obtain a percent methylation at each GpG site within the PGR product.

61

K562/S

100

80

60 40 20

K562/R

-228 -162 -125

100

80 H 60 40 20

-90 -JO 24 93

HL60/S

-228

100

80

60

40 20

-162 -125 -90 -30 24 93

HL60/R

-228

100 80

60 40 20

-162 -125 -90 -30 24 93

-228 -162 -125 -90 -30 24 93

Figure 10. 5-methylcytosine detection within the dCK 5' CpG island in K562/S, K562/R, HL60/S, and HL60/R. The y-axis is the percent methylation detected (multiple clones of the PGR product were cloned and sequenced, n = 5) and the x-axis is the location relative to dCK transcription start site. At the top, the solid black line depicts schematically the region of dCK sodium bisulfite sequenced, with exon 1 of dCK shown as an open box.

62

AML #1 M r AML HDAC/D

AML #2 M r AML ara-C/D

AML #3 F AML 2nd relapse HDAC/D

AML #4 F r AML HDAC/M

AML #5 M r AML HDAC/M

AML #6 F AML relapse HDAC/D

AML #7 M r AML HDAC/D

AML #8 M AML relapse ara-C/D

Table 2. Suminary of the ara-C-resistant acute myeloid leukemia (AMD samples obtained for the studies presented in this chapter and chapter 4. All the patients obtained for study failed araC-based chemotherapeutic regimes. Abbreviations: AML = acute myeloid leukemia, M = male, F = female, HDAC = high dose cytosine arabinoside, ara-C = cytosine arabinoside, D = daunorubicin, and M = mitoxantrone.

63

AML #1

PBIi

100 -

80 t 60 -40 -20 : 0

-228-162-125 -90 -30 24 93 100 -80 -60 40 -20 • 0 I i

-228-163-125 -90 -30 24 93

AMI. #5

100 80 60 40 20 0

-228-162-125 -90 -30 24 93

100 : 100 80 • 80

AML #2 AML #6m 20 " 50 0 0

-228-162-125 -90 -30 24 93 228-162-125 -90 -30 24 93

100 •

*0 • 100 60 ^ 80

AML #3 : AML #7 4 20

0 • 0

-228-162-125 -90 -30 24 93 -228-162-125 -90 -30 24 93

100 -

~ go * AML *4 S : *ML tSM 1

40 - " ̂ 20 • 20 • »

0 — 0 *

-228-162-125 -90 -30 24 93 -228-162-125 -90 -30 24 93

Figure 11. The sodium bisulfite sequencing of the dCK 5' CpG island in normal human peripheral blood lymphocytes (PBL) and ara-C-resistant adult acute myeloid leukemia (AML) patients. The y-axis is percent methylation and the x-axis is the location relative to the dCK transcription start site.

64

CRJiPTBR 4 - OKTSmcniATZOII OF 5-lfBTHTX.CTTOSZIfS

mrLUENCS att pis ahd pi6 kxprksszon

Es^ablxshad hiT«n lttuk«aixa call linss

After our initial studies on deoxycytidine kinase

(dCK) did identify a role for DNA methylation, we shifted

the focus to tumor suppressor, or genes capable of

preventing the conversion of normal cells to cancer cells,

that were hypermethylated. Fortunately, pl5 and pl6

presented an interesting situation to studying alterations

in DNA methylation. In 1997 Herman reported that Southern

blots (a technique that only determined the methylation

status of one pl5 CpG site) detected pl5 methylation in 88%

of AML patients (n = 60) but an absence of pl6 methylation.

These findings were surprising because pl6 is frequently

methylated in melanoma, breast, colon, lung, and Non-

Hodgkin's lymphoma whereas pl5 is only methylated in AML

and T-ALL. Thus, we already had AML patient samples with

which to do a detailed study of the pl5 and pl6 methylation

patterns in AML patients and cell lines. The initial

studies used established human cell lines to detect

methylation patterns of both pl5 and pl6.

65

We hypothesized that DNA hypermethylation was

associated with decreased expression of pl5 and/or pl6 in

leukemia cells. To address whether DNA methylation of the

pl5 or pl6 5' CpG islands was associated with gene

inactivation we obtained the following established human

leukemia cell lines: U937, monocytic leukemia (Nilsson and

Sundstrom 1974), KG-1, acute myeloid leukemia (Koeffler and

Golde 1978), and KG-la, a less differentiated variant of

KG-1 obtained after subcultivation of KG-1 (Koeffler et al

1980). In addition, the acute myeloid leukemia cell line

HL60/S, in Chapter 3, was also used here.

KG-1 was originally obtained from a patient with AML.

After subcultivation of KG-1, a phenotypically distinct

subline, designated KG-la, emerged. KG-1 and KG-la are an

interesting pair of cell lines. Though both KG-1 and KG-la

originated from one AML patient, some of the phenotypic

differences between KG-la and KG-1 are: (1) KG-la is less

differentiated than KG-1 based on the cellular markers

present on the cells surface, (2) KG-la will form colonies

in soft agar, but KG-1 does not, (3) KG-1 differentiates in

response to phorbol ester treatment while KG-la does not,

and (4) KG-1 is GM-CSF responsive but KG-la is not. The

four myeloid leukemia cell lines, U937, HL60, KG-1, and KG-

66

la were used to determine pl5 and pl6 (1) mRNA by RT-PCR,

(2) protein by immunoblotting, and (3) DNA methylation

levels by sodium bisulfite sequencing. In addition, four

other cell lines were used as controls. HaCaT, a human

keratinocyte cell line, served as a positive control for

pl5 mRNA and protein detection (Boukamp et al 1988). RHEK-

1, a human keratinocyte cell line, served as a positive

control for pl6 protein detection (Rhim et al 1985).

Melanoma UACC612, derived at the Arizona Cancer Center from

a patient with melanoma, served as a positive control for

pl6 methylation detection. Finally, Jurkat, a human T-cell

acute lymphocytic leukemia (T-ALL) cell line served as a

negative control for both pl5 and pl6 as it contains a

homozygous deletion of both pl5 and pl6 at chromosome 9p21

(Neuveut et al 1998). The cell lines and pl5 and pl6 RT-

PCR and immunoblotting results are summarized in table 1.

pl5 and pl6 mRNA. and protein atudx^a in leukemia cell lines

The established human leukemia cell lines were used to

determine if DNA methylation was associated with a loss of

pl5 or pl6 mRNA and protein. We determined pl5 and pl6

mRNA presence by RT-PCR. U937, HL60, HaCaT, and melanoma

UACC612 all had detectable pl5 mRNA by RT-PCR as shown in

67

figure 11. In contrast, pl5 mRNA was not detected by RT-

PCR in Jurkat, KG-1, and KG-la. In all samples Histone 3.3

was detected by RT-PCR as a control for RNA integrity.

Immunoblotting was used to detect pl5 and pl6 protein in

the same cell lines. pl5 protein was detectable in U937,

HL60, HaCaT, and melanoma UACC612, while Jurkat, KG-1, and

KG-la all lacked detectable pl5 protein, shown in figure

12. In addition to pl5, we also determined the status of

pl6 mRNA and protein. pl6 mRNA was detected in KG-1, KG-

la, and HL60 but not in Jurkat, U937, HaCaT, or melanoma

UACC612, shown in figure 12. pl6 protein was detected in

KG-1 and KG-la, but not HL60, U937, Jurkat, HaCaT, or

melanoma UACC612, see figure 13. These results indicate

that pl5 mRNA and protein were not detectable in Jurkat,

KG-1 or KG-la, but both pl5 mRNA and protein were detected

in U937, HL60, melanoma UACC612, and HaCaT. In the case of

pl6, pl6 mRNA and protein were not detected in Jurkat,

U937, melanoma UACC612, HaCaT, while HL60, KG-1, and KG-la

had detectable pl6 mRNA (see Table 1 in Chapter 1 for a

summary).

68

M 8

Figure 12. RT-PCR detection of pl5, pl6, and Histone 3.3 mRNA by ethidium bromide staining of a 2% agarose gel. The lanes are: M = marker, 1 = mock, no RNA, 2 = Jurkat, 3 = KG-la, 4 = KG-1, 5 = U937, 6 = HL60, 7 = melanoma UACC612, and 8 = HaCaT. For pl5 and pl6, 1 (ig of total RNA was reverse transcribed and amplified for 33 cycles. Histone 3.3, 100 ng total RNA amplified for 25 cycles, served as a control for RNA integrity.

69

16.7 Kd 6.7 Kd

1 2 3 4 5 6 7 8

pl5

16.7 Kd 6.7 Kd

•pi 6

Figure 13. Detection of pl5 and pl6 protein in Jurkat (lane 1), KG-la (lane 2), KG-1 (lane 3), U937 (lane 4) HL60 (lane 5), melanoma UACC612 (lane 6), HaCaT (lane 7), and positive controls, recombinant pl5 and RHEK-1 pl6 (lane 8). Each sample, excluding the positive controls, contained 0.25 mg of protein resolved by SDS-PAGE on a 15% acrylamide gel. The arrows at 16.7 and 6.7 kilodaltons show migration of protein standards.

70

Definition o£ th« pl5 msxleal proao-ter In HaCaT calls

To determine the region of the pl5 5' CpG island

responsible for pl5 gene activity, three deletion

constructs of the pl5 promoter were generated and inserted

5' of the chloramphenicol acetyltransferase (CAT) reporter

gene, see figure 13. The pl5 promoter constructs are:

plSPSTl from -1177 to +92, pl5PST2 from -448 to +92, and

pl5PST3 from -126 to +92, in all cases the numbering refers

to position relative to the pl5 transcription start site.

The results, shown in figure 14, demonstrate that pl5PST2

promoter activity in HaCaT was ~3.5 times greater than

pl5PSTl, and ~4.3 times greater than pl5PST3. These

results indicate that the region most relevant to pl5

transcriptional activity is located within the region from

-448 to +92 relative to the pl5 transcription start site.

Regions of the pl5 promoter further 5' of -448 are not

likely responsible for pl5 transcriptional activity, and in

fact may be inhibitory. Based on these results we chose to

sodium bisulfite sequence the pl5 5' CpG island from -440

to +474.

71

plSPSTl -1177 pl5PST2 -448 ̂ mhh^mhh^hm-i-92 pl5PST3 "126 mmmmm'^92 Sodiism bisxilfite aAi-niArt^-i tirr —440 +474 sequencing

20

basic SV40 PSTl PST2 PST3

Figure 14. CAT reporter contructs of the pl5 5' region were transiently transfected into HaCaT. Three constructs containing pieces of the pl5 promoter were cloned into the pCAT vector. pl5PST2, from -448 to +92 relative to pl5 transcription start site has the highest activity normalized to I3GAL activity and total protein isolated. As shown, the region sodium bisulfite sequenced overlaps most of P15PST2 (n = 3).

72

DMA mathyla^on mapping o£ pl5 and pl6 5' CpG Islands

In established human laukamxa call Unas, normal hi,man bona

marrow (MBM) , and AML patients

The pl5 CpG island was sodium bisulfite sequenced from

-440 to +474 relative to the transcription start site; this

region contains 80 CpG sites. The cell lines U937, HL60,

melanoma UACC612, and HaCaT were all primarily unmethylated

in the pl5 CpG island, see figure 15, and all had

detectable pl5 mRNA and protein. The other cell lines

analyzed, Jurkat, KG-1, and KG-la did not have detectable

pl5 mRNA or protein. Jurkat methylation was not determined

because pl5 and pl6 are both deleted in this T-ALL cell

line. In the case of KG-1 and KG-la, two distinct modes of

aberrant methylation of the pl5 CpG island were identified.

KG-1 had a variegated pattern with 23 of 80 CpG sites >40%

methylated throughout the pl5 CpG island. All the alleles

sequenced were partially methylated consistent with

methylation of both pl5 alleles in KG-1. The other form of

methylation, observed in KG-la, was complete methylation

with >80% methylation in 75 of the 80 CpGs sites

distributed throughout the pl5 CpG island. These results

provide in vitro evidence that variegated methylation and

complete methylation of the pl5 5' CpG island observed in

73

KG-1 and KG-la are both associated with transcriptional

silencing of pl5.

In addition to pl5, we also determined the 5-

methylcytosine content of the pl6 5' CpG island in the cell

lines described above- The pl6 CpG island was sodium

bisulfite sequenced from -552 to +156 relative to the

transcription start site; this region contains 53 CpGs.

KG-1, KG-la, and HL60, the three AML cell lines that were

positive for pl6 mRNA, all had only low DNA methylation at

the pl6 CpG island, see figure 15. Similar to the study of

Herman at al (1996) where Q937 was methylated at a Sacll

site in pl6, we detected 80% methylation of U937 in the 3'

region of pl6 from +92 to +156, which contains the Sacll

site. The 5' region of pl6 in U937, however, was only 20%

methylated from -404 to +92. We could not detect pl6 mRNA

or protein in HaCaT. In addition, HaCaT contained >60%

methylation in 5 of 7 sites from -461 to -380, and also

from +29 to +53 in the pl6 5' CpG island. A recent study

corroborates our finding that pi6 is not present in HaCaT

(Munro et al 1999). Melanoma UACC612 lacked detectable pl6

mRNA or protein, and contained >80% methylation in 51 of 53

CpG sites in the pl6 CpG island. In summary, the results

obtained from sodium bisulfite sequencing indicate that

74

while the pl6 CpG island displays more complex regional

patterns of methylation in vitro than the pl5 CpG island

(see U937 and HaCaT figure 15), an association between pl6

gene inactivation in vitro and DNA methylation was observed

in melanoma UACC612.

We also determined the 5-methylcytosine content of the

5' CpG islands of pl5 and pl6 in 2 normal human bone marrow

samples (NBM) and 8 cytosine-arabinoside (araC)-resistant

adult acute myeloid leukemia patients. In the 2 NBM samples

pl5 and pl6 were both predominantly unmethylated, see

figure 16, part 1. pl6 had only 1 methylated cytosine of

the_ 1, 060 CpGs sequenced or ~0.1% of all sites (n of 10 per

sample), while pl5 had 37 methylated cytosines of the 1,600

CpGs sequenced or -2.3% of all sites (n of 10 per sample).

In this study, the pl5 CpG island of NBM was ~25 times more

likely to be methylated at any given CpG compared to the

pl6 CpG island, however, overall both were largely

unmethylated. These results show that the pl5 and pl6 5'

CpG islands contain very low levels of methylation in NBM,

and are in accordance with other studies that have not

found DNA methylation in the 5' CpG islands of genes in

normal human tissue (Fryxell et al 1999).

75

The ara-C-resistant acute myeloid leukemia (AML)

patients had examples of all three types of methylation at

the pl5 CpG island described earlier in normal human bone

marrow (NBM) and the human cell lines KG-1 and KG-la.

Patients #6 and #7 were almost completely unmethylated;

combined patients #6 and #7 had ~2.9% of all CpG sites

methylated (n of 5 per patient) in similar fashion to NBM,

see figure 16, part 2. Patients #1, #2, #4, #5, and #8

displayed a variegated pattern throughout the entire pl5

CpG island similar to the pattern observed in KG-1, see

figure 16. Overall, of the 80 CpG sites analyzed in the

pl5 CpG island, >40% methylation was detected at 12 sites

in patient #1, 20 sites in patient #2, 33 sites in patient

#4, 26 sites in patient #5, and 15 sites in patient #8.

Finally, patient #3 (the only patient of the 8 in this

study that was in 2"*^ relapse) had almost complete

methylation of the pl5 CpG island with 78 of 80 CpGs > 75%

methylated, similar to KG-la.

The pl6 CpG island, in contrast to the pl5 CpG island,

contained only 8 methylated cytosines of the 2,120 CpG

sites analyzed in the 8 AML patients, or ~0.4% (n of 5 per

patient), a result similar to the methylation levels

detected in NBM, see figure 16 parts 1 and 2. In

76

conclusion, the results obtained from sodium bisulfite

sequencing the 8 AML patients showed aberrant methylation

at the pl5 5' CpG island in 75% of the patients, but only

minimal methylation at the adjacent pl6 5' CpG island.

Further, the methylation patterns of the pl5 5' CpG island

in AML were found to extend throughout the region analyzed

from +474 to -440, and can be categorized as either (1)

minimal methylation (2 of 8) (2) variegated methylation (5

of 8) , or (3) complete methylation (1 of 8) .

77

10 0

80

60 •

40

20

0 1 BL60

-440-151-75 28 113 233 322 416

100-

8 0 -

60 :

40 •

2 0 -

0 1 -552 -344 -177 -19 50 140

100

80

60

40

20

0 J L -440-151-75 28 113 233 322 416

100-|

8 0

60

4 0 1 1 • i 1 KG—1

20

-440-151-75 28 113 233 322 416 552 -344 -177 -19 50 140

100

80

60

40

20

0

100

80 •

60 •

40 •

20 •

0

1 0 0 -

8 0 -

60 •

40 -

20 -

0

K6-l«

-440-151-75 28 113 233 322 416

100-

80-^ 60-;

40

20

0 -552 -344 -177 -19 50 140

i -440-151-75 28 113 233 322 416

-440-151-75 28 113 233 322 416

Ml 100-

OACC 80 1

612 6o] 40 1 201

0 ' 100-

HaCaT 8 0 -1 60 ii 40 1 20 j 0

-552 -344 -177 -19 50 140

Figure 15. Methylation analysis of pl5 & pl6 in cell lines.

78

pl5 pl6

100 80 60

40

20 0

100 80

60 40 20

0

100

80

60 40 20

0

NBM «1

kjLA A A -440-151-75 28 113 233 322 416

100

80

60 :

40 •

A °-552 -344 -177 -19 50 140

100^

iLL. -A 4- -A—i -440-151-75 28 113 233 322 416

80^ 60-

NBM «2 40 • 2 0 •

0 -552 -344 -177 -19 50 140 100-

8 0 -

6 0 -

MfL *1 4 0 -2 0 1

-440-151-75 28 113 233 322 416 ^ -552 -344 -177 -19 50 140 100

80 •

6 0 -

MIL *2 20

-552 -344 -177 -19 50 140 100:

80^

-440-151-75 28 113 233 322 416

MIL #3 i 40 1

2 0 1

0 552 -344 -177 -19 50 140

Figure 16, part 1. Sodium bisulfite sequencing of pl5 and pl6 in two normal bone marrow samples (NBM) and 3 of the 8 adult acute myeloid leukemia (AML) patients.

79

lOO:

80 •

60 40 20

0 -440-151-75 28 113 233 322 416

100~

MiL «4 80-

60] 40 • 201

0 -552 -344 -177 -19 50 140

100 80 60 40 20

0

100 MO. #5 80

60

40 20

-440-151-75 28 113 233 322 416 0 -552 -344 -177 -19 50 140

100 80 •

6 0 •

40 • 20 0 1

100"

AML «6 80 60 40'

14 A- 20^__| -440-151-75 28 113 233 322 416 0-552 -344 -177 -19 50 140

100"

80 '

60 •

40 1 20 I 0

100"

MIL «7 8 0 '

60 -

40 1

J A_i i -440-151-75 28 113 233 322 416 -552 -344 -177 -19 50 140

100"

MIL *8 : 601

440-151-75 28 113 233 322 416

40 1

L -552 -344 -177 -19 50 140

Figure 16, part 2. Sodium bisulfite sequencing of pl5 and. pl6 in the remaining 5 adult acute myeloid leukemia (AML) patients.

80

NBM#1

GO •DOO OOO O «D O ooa ID O 0<D OO o o« mtD •o o* OO «DOO OOO O €D o OOJ D O 0<D OO O OO OOO OO OO

OO «DO* OOO O CD o OOO D O ooa eo O OO OOO OO OO «o •DOO OOO O «D o o«a ID O oa» OO O OO OOD OO OO GO «DOO OOO O «D o oa D O 0<D OO O OO OOD OO OO OO «DOO OOO O €D O 009 ID O OOD OO O OO OOO OO OO

OO «B>00 OOO O €D O 003 ID O oa> OO O OO OOO OO OO OO •DOO OCO O <D O OOO 09 O OOO OO O OO OOD OO OO

AML#5

•D mmoo oamo o 0«D • om OO o •• COD •o oo 00 mooo oaoo CD o OOOD o oca OO O OO OOD oo oo «> mooo oaoo CD • • (» • oca 3« o mm mom oo oo «o •DOO oaoo CD o OOOD o OO •O O OO mm •• •• •0 mmmo ooM m o 0«fl» • o<D OO • •• mo •o 00 cm mtmm mmo CD o oa» • • a» OO o •• mo •• oo m mmmo mcmm « o 0<MD • OOD OO • •• mo mm oo

cm mmmm ocmm CD • • CH» • mm •• o •• mam om oo

-14 +385

Figure 17. Individual sodium bisulfite sequences from 1 normal human bone marrow (NBM#1), and 2 AML patients (AML#3 and AML#5). The open circles indicate unmethylated 5'-CG-3' sites and the closed circles indicate methylated 5'-CG-3' sites. The variegated pattern of pl5 methylation pattern is shown in patient #5, and similar results were obtained from AML patients #1, #2, #4, and #8. On the bottom, the position relative to pl5 transcription start site is indicated.

81

CHAPTBR 5 - niTRODUCTION OT P15 AMD P16

INTO TBX T-ALL CELL LZME JURKAT

Stabla ovarM^rassion ot pl5 or pl6 xnte Jurkat Z:

•stablxaluMn ̂ of pl5 and pi6 poal^v* aubclonas

Jurkat is a human T-cell adult acute lymphocytic

leukemia (T-ALL) cell line. In order to confirm previous

reports that Jurkat lacks pl5 and pl6, we performed PGR

that overlaps either pl5 exon 1 or pl6 exon 1, see figure

18. This result corroborated previous reports that Jurkat

is pl5 and pl6 negative due to homozygous deletion at

chromosome 9p21 (Neuveut et al 1998). As demonstrated in

chapter 4, pl5 but not pl6 is methylated in AML. In

addition to AML, methylation of pl5 but not pl6, as well as

homozygous deletion of both pl5 and pl6 (as is the case

with Jurkat), occurs in T-ALL (Batova et al 1997), To

attempt to identify a role for pl5 in leukemogenesis, pl5

or pl6 were introduced into the T-ALL cell line Jurkat-

pl5 or pl6 introduction may result in cell death or a

dramatic decrease in cell growth, for this reason we began

by trying to establish inducible expression of pl5 or pl6.

To achieve inducible expression we used the tetracycline

82

lOObp PBL JE^

lOObp

p15

p16

Figure 18. The PGR for portions of exon 1 of both pl5 and pi6 was performed with normal peripheral blood lymphocyte (PBL) DNA and Jurkat Tet-Off (J) DNA. As indicated with the arrows, PGR products were detected in PBL for both pl5 and pl6 but not in Jurkat Tet-Off consistent with the presence of a homozygous deletion of both pl5 and pl6 in Jurkat.

83

inducible expression system originally described by Gossen

and Bujard (1992).

The cell line Jurkat Tet-Off was purchased along with

the necessary plasmids from Clontech. Jurkat Tet-Off was

generated by stable expression of a tetracycline responsive

protein fused to the VP16 transactivation domain (tetR-

VP16) in Jurkat. With the addition of tetracycline (tet)

or doxycyline (dox) tetR-VP16 no longer transactivates any

gene introduced with a 5' tetracycline-responsive element

(TRE), see figure 19. After obtaining Jurkat Tet-Off, an

initial experiment was performed to confirm that tetR-VP16

was functional. We transiently transfected a green

fluorescent protein (GFP) plasmid with a 5' TRE into Jurkat

Tet-Off. The transfected cells were then cultured in the

presence of 0.001 to 1000 ng/mL dox. The result, shown in

figure 20, demonstrated that tetR-VP16 was inhibited by

increasing dox concentration. We next attempted to

establish stable inducible expression of pl5 and pl6 in

Jurkat Tet-Off cells. Two independent strategies of

electroportion were attempted to establish stable

transfection into Jurkat Tet-Off: (1) two plasmids, the

hygromycin drug resistance gene, pTK-Hyg, plus the pl5 cDNA

84

Inttgrata^ copy •! pT•^Off rcfiiatar piasiRid

i-TctarDox)

TcMrOcK)

TrancriMNs

lalaflraM copy of pTRE rospoaso plasm ii

Figure 19. Explanation of the tetracycline inducible expression system described by Gossen and Bujard in 1992. The TetR-VP16 fusion protein is stably integrated in Jurkat Tet-Off. Introduction of a gene containing a 5' TRE can be induced by the removal of tetracycline or doxycyline.

85

% 6FP-I-Jurkat: | q -Tet-Off

0.4 -

0.001 0.01 0.1 1 10 100 1000 10000

doxycylxne ng/mL

Figure 20. A doxycyline responsive GFP vector was transiently transfected into Jurkat Tet-Off cells. Increasing concentrations of doxycyline (0.001 ng/itiL to 1000 ng/rtiL) decreased the number of GFP positive cells as determined by flow-assisted cytometry (FACS) analysis. This demonstrated that Jurkat Tet-Off contains a functional tetR-VP16 protein.

86

with a 5' TRE, plSpTRE, or (2) the hygromycin drug

resistance gene subcloned into the plSpTRE plasmid to

generate one plasmid, pTKHygplSpTRE. The electroporated

cells were selected for 3 weeks by limiting dilution in the

presence of 400 ng/mL hygromycin. The use of the 2 separate

plasmids was used by Bujard and Gossen (1992) in defining

this system in HeLa cells, and is the procedure recommended

by Clontech (the single plasmid containing the TRE and

hygromycin resistance gene required assembly). The idea to

use a single plasmid came from the few reports in the

literature where the tetracycline inducible expression

system was used with Jurkat cells (Kwon et al 1998).

As shown in table 3, only 1 of 36 independent clones

obtained from limiting dilution of the Jurkat Tet-Off

transfected cells using the two separate plasmids actually

expressed pl5. In contrast, the single plasmid

electroporation yielded 11 of 24 pl5 mRNA positive clones.

As figure 21 illustates, though, the pl5 protein levels

were not shut off in the presence of 1 ng/mL of dox (all

selection was performed in the presence of dox and separate

clones grown in absence of dox were used to determine the

pl5 protein levels). In summary, the results obtained

87

suggest that inducible expression is difficult to obtain in

Jurkat cells likely due to the requirement of a single

plasmid transfection. The clonal sublines of Jurkat were

treated as stable overexpressors of either pl5 or pl6, see

figure 22.

88

+ - + - + - + - p i s

p15

Figure 21. The clonal populations that were hygromycin-resistant and pl5 itiRNA positive without doxycyline were grown in the presence (1 ng/mL) or absence of doxycyline. The pl5 protein levels of the 12 clones were then determined by Western blot, 100 ng per sample. As shown, the expression of pl5 was not inducible.

89

Number of 24 36 clones pl5 DNA 17 of 24 22 of 36 positive pl5 RNA 11 of 24 1 of 36 positive Inducible 0 of 11 0 of 1 expression

Table 3. Summary of the results of the two approaches to obtaining pl5 positive Jurkat Tet-Off cells. The Clontech recommended protocol of two plasmids yielded only 1 of 3 6 pl5 mRNA positive clones. In constrast, the single plasmid, pTKHygplSpTRE, yielded 11 of 24 pl5 positive clones. Our analysis did not show any clones that were inducible due to the high level of "leaky" expression in the presence of doxycyline (l|ig/mL), see figure 20.

90

T-O Pl5 pl6

pl5

pl6 -M

Figure 22. Establishment of multiple clones of Jurkat Tet-Off that stably overexpress either pl5 or pl6. A Western blot was performed with 100 ng of protein per sample, a pl5 fusion protein served as a positive control for pl5 detection, and RHEK-1, a human keratinocyte cell line, served as a positive control for pl6 detection.

91

Stable overttxpresslon of pl5 or pl6 xn Jurkat ZI: r«duc«d

groirth of pl5 positive cells and unchanged axa-C and

daianonabxcln sensitivity

The growth of the pl5 or pl6 positive clones of Jurkat

was measured by plating 400,000 cells per well in 6-well

plates and counting total cell number each day for 6 days.

The results, shown in figure 23, revealed that pl5 clones

grew slower than the pl6 clones or hygromycin only selected

cell line. Interestingly, after the initial slow growth,

the pl5 positive clones displayed a similar rate of growth

from day 4 to day 6. This may represent a cytokine-

dependent growth rate that is slower to "turn-on" in the

pl5 positive clones.

The decreased growth in the pl5 positive clones was

further confirmed by using the MTS assay, which determines

metabolic activity. In the MTS assay, 8,000 cells were

plated out per well in 96-well plates and allowed to grow

for 5 days. The results, shown in figure 24, indicate a

statistically significant decrease in growth only in the

pl5 clones (paired T-test, n = 3, T = 7.24, p = 0.0185).

To determine why the pl5 cells were growing slower we

performed: (1) a Western blot to determine the

phosphorylation status of retinoblastoma (pRb) (2) cell

92

cycle analysis by flow-assisted cell sorting (FACS) with

propidium iodide (PI) staining, and (3) apoptosis analysis

with annexin V/PI FACS staining. The phosphorylation of

retinoblastoma was not altered in either the pl5 or pl6

clones (data not shown)- In addition no differences in the

% growth

4500

4000

3500

3000

2500

2000

1500

1000

500

0

^ "

• •

- -

-i--

/ . . - -

- V

. .V

^ ' .

m

^ T — 1

2 3 4 5

days in culture

6

pTKHgy p15

p16

Figure 23. Cells were plated in 6-well plates at 400,000 cells in 4 mLs of media and allowed to grow for 6 days. Cell counts were performed on days 2-6. The y-axis is percent of cell growth, and the x-axis is days in culture. A hyrogromycin only selected clone, pTK-Hyg, and 2 clones each of pl5 and pl6 are summarized. As shown, pl5 clones had the slowest growth rate (n = 2, one representative result is shown).

93

140

120

0) |3 100 (0

80 -

•S 60

40

20

T

- *

T

-

" • '

" r

1 '

Jurkat Tet-Off pIS-i- p16-i-

Figure 24. Equal cell numbers, 8,000 cells per well, were plated out in a 96-well plate and allowed to grow for 5 days. Metabolic activity was determined at day 5 using the MTS assay (n = 3, the error bars show the standard deviation). The asterisk (*) indicates statistical significance using the Sigma Plot software, paired T-test (paired T-test, n =3, T = 7.24, p = 0.0185).

94

cell cycle profile (Gl, S-phase, and G2/M) were observed in

the pl5 or pl6 positive clones (data not shown). In the

annexin V staining experiments, increased apoptosis and

necrosis was detected in one of the pl5 clones, shown in

figure 25 (not all pl5 positive clones showed an equal

increase, only the most dramatic clone is shown). These

results suggest that pl5 introduction into Jurkat decreases

growth due to increased cell death.

All 8 AML samples used to describe the aberrant

methylation of pl5 in 6 of the 8 AML cases in chapter 4

were ara-C-resistant. Thus, loss of pl5 or pl6 in Jurkat

may represent a mechanism of drug resistance acquired after

drug treatment. To determine if ara-C or daunorubicin, two

drugs currently used clinically to treat AML and T-ALL,

would have increased efficacy in the pl5 or pl6 positive

clones of Jurkat, we performed an MTS assay with ara-C or

daunorubicin doses from 1 nM to 1000 nM. The results,

shown in figure 26, indicate that pl5 or pl6 presence in

Jurkat cells does not alter sensitivity to ara-C or

daunorubicin. The IC50 values of ara-C treatment of Jurkat

Tet-Off, pl5, and pl6 for were 44.8 nM, 45.1 nM, and 44.9

nM respectively. These results suggest that pl5 or pl6

loss occurs independent of drug treatment.

%of total cells

% necrotic

% apoptotic

T-O Hygro pl5 pl6

Figure 25. Annexin V and propidium iodide staining were used to determine the percent of cells that were apoptotic shown in blue, and the percent of cells that were necrotic shown in black. Flow-assisted cytometry (FACS) was used and 10,000 events per sample were scored (n = 2, one representative experiment is shown).

%

AraC Dose Response

0.000001

>1 a. ̂ ̂̂ ^

« 0.6

A—p16

0.00001 0.0001

Molar Concentration of AraC

0.001

Tet-Off

Daunorubicin Dose Response

.2 £ 3 CO

u

0.000001 0.00001 0.0001

Molar Concentration of Daunorubicin

0.001

Tet-Off pis p16

Figure 26. MTS assay of the relative sensitivity of Jurkat Tet-Off, a pl5 clone, and pl6 clone to ara-C and daunorubicin. The parent cell line, Jurkat Tet-Off is shown in blue, the pl5 clone is shown in pink, and the pl6 clone is shown in purple (similar results were obtained for a total of 3 clones each for both pl5 and pl6, n = 3).

97

St:able ovarsxprttsaxon of pl5 or pl6 In Jurkat ZIZ: cDHA

mxcroarray analysis of 5700 gttn«s rsvaals tlia^ pl5 and pl6

differ froa Jurkat bu^ ar« similar te aach other

To obtain a bird's eye view of the alterations that

occurred in Jurkat Tet-Off after pl5 or pl6 introduction,

we performed expression analysis on ~5700 cDNAs spotted

onto a microscope slide, referred to as microarray. As

noted in the previous section a decrease in the growth of

the pl5 positive clones was found. This suggested that

possibly there was a pl5 specific function distinct from

pi6. The use of microarray allowed us to determine the

expression changes that occurred in the pl5 and pl6

positive Jurkat cells.

An example of the results obtained when the mRNA from

a pl5 positive clone was labeled red with Cy3-dCTP and

Jurkat Tet-Off mRNA was labeled green with Cy5-dCTP is

shown in figure 27. A number of cDNAs, ~20 showed altered

expression in all three pl5 or all three pl6 clones. pl5

and pl6 expression profiles were distinguishable from

Jurkat Tet-Off. Interestingly, and counter to the growth

studies, the pl5 and pl6 positive clones had similar

expression changes from the parent cell line Jurkat Tet-

Off. Specifically, we performed northern blot analysis to

98

confirm the expression changes determined using microarray

on the following 5 genes (see table 4): (1) the tyrosine

phosphatase PTPNl; (2) heparin-binding epidermal growth

factor-like growth factor; HB-EGF, (3) the anti-apototic

BCL-2 family gene, MCLl; (4) the pro-apoptotic gene

BCL2/adenovirus ElB 19kD-interacting protein 3, BNIP3; and

(5) the interferon-gamma inducible transcription factor,

IRF-1. In addition, GAPDH mRNA levels were determined for

each blot to ensure equal loading and also for use in

quantitative expression levels. The northern blot results,

shown in figure 28, confirmed the miroarray data. The

expression levels were quantitated using the Stratagene

Eagle-eye software, normalized to GAPDH levels, and the

data obtained from microarray and northern blots are

summarized in figure 29. The results show that microarray

data and northern blot data were similar. The total number

of genes with altered expression in pl5 and pl6 was -20 or

~0.4% of all the genes assayed by microarray (several of

which were ESTs of unknown function). The expression

changes in pl5 and pl6 were concordant. These results

suggest that pl5 and pl6 are functionally equivalent and

interact in the same genetic networks.

99

The red spot below corresponds to BNIP3, accession namber AA446839, indicating a teck of CyS-CTP (green) bnt presence of Cy3-CTP (r^) from the parent ccU line cDNA. Expression of BN1P3 is decreased in pl5/pl6 Jnrkat cells.

Figure 27. A example of the use of a 5,700 cDNA microarray to determine the alterations in expression between pl5 or pl6 and the parent cell line Jurkat. The parent cell line mRNA was labeled red with Cy5-dCTP and the pl5 or pi6 clones were labeled green with Cy3-dCTP. A red or green color indicates differential expression, while yellow indicates similar expression levels.

100

CHANGE IN ABBREVIATION FUNCTION EXPRESSION

IN pl5/pl6 BNIP3 Pro-apoptotic Decreased HB-EGF Growth factor Increased IRF-1 Transcription

factor Increased MCLl Anti-

apoptotic Increased Tyrosine

PTPNl phosphatase Increased

Table 4, A list of the genes that were chosen for further analysis from the microarray data.

lOl

T-O Hyg pl5 pl6

BNIP3 9 •

GAPDH

HB-EGF

GAPDH

MCLl

GAPDH

IRF-1

GAPDH

PTPNl

GAPDH

Figure 28. Northern analysis using 20 (ig of otal RNA per lane. The genes tested were selected based on microarray data of 3 independent pl5 and pl6 clones of Jurkat.

102

• = Microarray result H » Northern result

Fold expression change vs.

Jurkat Tet-Off

B3 HB ML IR PT R^ HR ML IR PT

pl5 pl6

Figure 29. Summary of the results obtained with microarray, in white, and Northern blots, in black. Genes studied: B3 = BNIP3, a pro-apoptotic gene; HB = HB-EGF, a mitogenic gene; ML = MCLl, an anti-apoptotic gene; IR = IRF-1 an interferon-responsive transcription factor; and PT = PTPNl, a protein tyrosine phosphatase.

103

CBAPTKR 6 - DISCUSSION

Aberrant Dim of th* pl5 5' CpG Island occurs iJi

the majority ot acuta Hyaloxd lanlrssii a (AML) patiants and

might dysragulata normal haeatopoietic dlf£arantlatlon

The hypothesis of the preceding experiments is that

hypermethylation of 5' CpG islands is associated with

transcriptional silencing of the corresponding gene and

participates in either the emergence of drug resistance or

the conversion of normal cells to cancer cells. The

hypothesis that decreased dCK activity, a mechanism of drug

resistance, was mediated by hypermethylation of the 5'

maximal promoter of dCK was tested and disproved.

Next, the hypothesis shifted to the role of DNA

methylation in the transcriptional silencing of pl5 and

pl6, representing a mechanism of avoiding normal tumor

surveillance and promoting the conversion of normal cells

to cancer cells.

The results obtained from studying the DNA methylation

patterns in leukemia cell lines and AML patients indicate

that while pl6 was not aberrantly methylated in the

leukemia cell lines or the AML patients, the aberrant

methylation of pl5 occurred both in vitro and in vivo. Two

104

distinct modes of aberrant pl5 methylation, variegated

methylation and complete methylation, were detected both in

vitro and in vivo. KG-1, an AML cell line, had variegated

methylation of pl5 associated with no detectable pl5 mRNA

or protein, and KG-la a subclone of KG-1 had complete

methylation of pl5 also associated with no detectable pl5

mRNA or protein. Six of the eight AML patients studied had

aberrant methylation of pl5, five of eight, 62.5%,

displayed a variegated pattern of pl5 methylation, and one

of eight, 12.5%, displayed a complete pattern of pl5

methylation. Thus, based on KG-1 and KG-la where

variegated and complete methylation of pl5 were both

associated with no detectable pl5 mRNA or protein, it is

reasonable to infer that in vivo aberrant DNA methylation

of pl5 in AML inactivates pl5 in 75% of AML patients.

The selective inactivation of pl5 but not pl6 is

surprising given that pl6 is located adjacent to pl5 on

chromosome 9p21 and shares >80% protein identity to pl5.

How such a situation arises in AML is not immediately

apparent. To try to understand whether pl5 has a specific

function that pl6 lacks we introduced pl5 or pl6 into the

pl5 and pl6 negative T-ALL cell line Jurkat.

lOS

We did detect reduced growth in the pl5 but not pl6

positive clones. In addition, while a 5,700 cDNA

microarray distinguished pl5 and pl6 positive clones from

the parent cell line, the pl5 and pl6 expression profiles

were very similar. This suggests, despite the decreased

growth seen only in the pl5 positive cells, that pl5 is

functionally equivalent to pl6. It is important to note

that while the use of microarray did provide enormous power

in understanding the expression changes in the pl5 or pl6

positive cells, it only measured -6% of all human genes.

It is possible th.at among the 94% of genes not studied

there are pl5 specific changes in expression that provide

evidence for a functional distinction between pl5 and pl6

that would explain the selective methylation of pl5. Also,

it may simply be the case that pl5 overexpression is

significantly higher than the pl6 expression levels.

Determination of the absolute amount of pl5 protein

relative to pl6 protein is not a trivial experiment because

of differences in antibody specificity. In summary, while

the growth of the pl5 clones suggested that pl5 may have

some functional independence from pl6, microarray

expression analysis of 5,700 cDNAs did not find any

evidence to support a pl5 specific function.

106

Several genes that were differentially expressed in

the pl5 and pl6 clones were identified from the microarray

data and confirmed by Northern blots. Among these, HB-EGF,

heparin-binding epidermal growth factor, has previously

been implicated in monocytic differentiation.

Specifically, phorbol ester treatment of HL60 results in

monocytic differentiation, associated with induced

expression of pl5 and HB-EGF (Schwaller et al 1997, Vinante

et al 1999). This provides a possible explanation for the

observed selective methylation of pl5 in AML. As shown in

figure 30, pl5 methylation may prevent the induction of pl5

that would normally mediate monocytic differentiaion by

triggering a cascade that induces other genes such as HB-

EGF. The blockade of this cascade may participate in the

genesis of acute myeloid leukemia (AML).

Di f f e ren t i a t i ng s i g n a l s

G r o w t h dys regu la ted i n A M L p l 5 me thy la ted ^ ^ ^

/ V / V

HB-EGF

107

Figure 30. A model of why pl5 is methylated in AML but pl6 is wild-type. A cytokine might direct normal hematopoietic differentiation by inducing pl5, which results in changes in the expression of genes such as HB-EGF. DNA methylation of pl5 might block this monocytic differentiation pathway.

108

Aberrant B«tbyla^on o f pl5 as a markar o f AML and

po^n^iaX targafc for noval drug traal«aiifca

To date, the predominant genetic and epigenetic

modifications described in acute myeloid leukemia (AML)

are: (1) the oncogenes ras and fms are mutated at

frequencies of ~30% and ~15% respectively (Bos et al 1987,

Tobal et al 1980) (2) several chromosomal translocations

occur that create fusion proteins; one of the most frequent

AMLl-ETO occurs in ~15% of AML patients (Look 1997), and

(3) DNA hypermethylation occurs in AML (Herman 1999).

Aberrant methylation of pl5 occurred in 6 of 8, or 75% of

the AML patients analyzed in this study. This percentage

is consistent with a larger study (n = 60) that found a

higher percentage, 88% of AML patients, that had aberrrant

methylation of pl5 (Herman 1997). Thus, pl5 methylation is

the most frequent alteration described to date in AML.

Aberrant methylation of pl5 is a potential marker for

AML. The detection of hypermethylation at the pl5 5' CpG

island could be important for: (1) the detection of AML,

(2) accurate diagnosis of AML, or (3) monitoring residual

disease after treatment. The high frequency of alteration

at the pl5 CpG island makes it a potentially important

future tool to monitor AML.

109

As shown simplistically in figure 31, the efficacy of

prokaryotic drugs, such as chloramphenicol, is explained by

their targeting of the unique prokaryotic structures that

differ from euJcaryotic structures, such as the ribosome in

the case of chloramphenicol. The treatment of cancer is

complex because both normal and cancerous cells are

eukaryotic and use the same basic cellular machinery. Most

cancer drugs in current use do not kill cancer cells based

on specfic defects in cancer cells. Ara-C and

daunorubicin, two drugs currently used to treat AML, kill

all rapidly dividing cells including normal cells.

Further, ara-C and daunorubicin treatment fails in ~40% of

all AML cases. Novel pharmaceutical drugs that target

specific defects in cancer cells might have higher efficacy

than current treatments.

Presently, 5-azacytidine is the only widely explored

inhibitor of DNA methylation. If demethylation of pl5

results in reactivation of pl5 and this puts AML into

remission, then this is a potential avenue for drug

exploration. A drug that demethylates pl5 would likely act

at numerous other gene promoters potentially resulting in

deliterious pleiotropic effects. Such a situation could be

avoided if it were possible to design drugs that only

no

demethylate specific genes such as pl5. Of course the

design of drugs that could specfically demethylate pl5 and

not other genes may not be possible. In summary, given the

frequency of aberrant methylation of pl5 in AML and the

need for targetted therapies to treat AML, reactivation of

pl5 by DNA methylation inhibitors represents an avenue for

potential drug discovery.

p r c k a ' a n s

111

Figure 31. Epigenetic changes such as DNA methylation represent a potential drug target in cancer. As prokaryotic cells demonstrate, specific alterations such as the completely different ribosomal architecture, provide a target for the selective killing of prokaryotic cells but not eukaryotic cells. Her-2 a receptor overexpressed in breast cancer is a paradigm case of the targeted pharmacology of cancer. DNA methylation is frequently altered in human cancer, thus it represents a target for novel pharmaceutical approaches.

112

G«n«ral po^antial fox nov«l th«r«p«u^e i.nterv«nti.on of

apxgene^c dimt»ctM xn bwmmxx cmnemx

Cancer is a genetic disease and the alterations that

occur in cancer can be classified as: (1) viral, (2)

chromosomal rearrangements, (3) mutation, and (4)

epigenetic/DNA methylation. As shown in table 5,

epigenetics/DNA methylation is the only category that both

has an endogenous role and is a potential target for cancer

drugs. In the case of viruses, no known endogenous role

exists. Chromosomal translocations of DNA are an

endogenous process used in V(D)J recombination, however

despite the occurrence of chromosomal translocations in

cancer it does not appear to be an avenue for drug

treatment. If the process of shuffling DNA that occurs

physiologically in V(D)J recombination could be harnessed

to any end, it is not apparent how this would be useful to

treat cancer. Mutation has no well documented endogenous

role within the lifespan of individual mammalian organisms.

It is entirely possible that mutation enables selection and

ultimately helps ensure the survival of a given species,

but within the lifetime of an organism there is no current

evidence that mutations in DNA have a physiological role.

In fact, mutation may be considered a complete failure of

113

the endogenous processes of DNA repair systems that attempt

to maintain DNA sequences intact within the organisms

lifespan. The case of epigenetics/DNA methylation is

unique. Because DNA methylation is a endogenous process

with physiological consequences, alterations in DNA

methylation represent an exciting possibility for future

cancer pharmacology that might be able to use the

endogenous methylation machinery to revert a cancer cell to

a normal cell. Again, as stated previously there are many

potential drawbacks of such a strategy such as the lack of

specificity in DNA methylation changes that could have

deleterious consequences. Nevertheless, based simply on

the existance of endogenous processes that both remove and

add methylation to DNA, particularly during development,

this is an area of cancer research worthy of future

investigations.

114

Viral No None/ Yes HTLV-1

Chromsomal Yes V(D) J No rearrangement rearrange­

ments/ AMLl-ETO

Mutation No None/p53 Gene therapy

Epigenetics, Yes Mammalian 5-aza, DNA development future

methylation /pl5 in AML drugs?

Table 5. A general classification of the alterations that occur in human cancer cells. DNA methylation represents an intriguing possibility because it is an endogenous process with physiological consequences. Thus pharmacological manipulation of the endogenous DNA methylation machinery might be able to revert cancer cells to normal cells. Currently, 5-aza = 5-azacytidine, is the only drug widely explored as an inhibitor of DNA methylation.

115

APPENDIX A. SUMnRT OF STODZSS TO TKST WBKTBSR KG-1 OR KG-

la CAN BE INDUCED WITHOUT DEMBTBTIATZON

One of the areas of research that was pursued but not

resolved involves whether the methylation of pl5 (observed

in the cell lines KG-1 and KG-la and in AML patients)

prevents the induction of pl5. From the original

description that TGF-P induces pl5 in HaCaT, it has been an

attractive idea that DNA methylation of pl5 blocks TGF-P

mediated pl5 induction. It has been published that

treatment with 5-azacytidine will result in reactivation of

pl5 in KG-la. The question here is whether an agent such

TGF-P, that is not a DNA methylation inhibitor, could induce

pl5.

First it was determined if leukemia cell lines also

show pl5 induction after TGF-p treatment. Because previous

studies demonstrated that HL60 lacks the TGF-p type II

receptor, HL60 was not included in this study. The cell

lines HaCaT (a positive control for TGF-P mediated induction

of pl5), U937, KG-1, and KG-la were tested. The results,

shown in figure A, show that only HaCaT had induced pl5

protein levels 24 hours after TGF-P (2ng/mL) treatment. It

could be argued that U937, KG-1, and KG-la are not

responsive to TGF-P, and this explains the lack of pl5

116

induction. To address this, cell cycle position v;as

determined by propidium iodide (PI) staining and flow-

assisted cell sorting (FACS), see figure B. This showed a

marked growth arrest only in HaCaT. Thus it may be the

case that the leukemia cell lines lack the necessary

signaling for TGF-P to induce pl5. Currently, there is no

precedent in the literature of a leukemia cell Xine that

shows induced pl5 after TGF-p treatment. Thus, these

results suggest that TGF-p mediated induction of pl5 may

only occur in specific cell types and not in myeloid cell

lines.

In addition to TGF-P inducing pl5 in HaCaT, it was

reported that PMA induces pl5 in HL60. Whether PMA would

also induce pl5 in U937, KG-1, and KG-la was determined.

The results shown at the bottom of figure A demonstrate

that both HL60 and U937 do induce pl5 in response to PMA

treatment, but KG-1 and KG-la, the two cell lines that

contain methylation of pl5, do not show pl5 induction (in

addition, no pl5 mRNA was detectable in KG-1 or KG-la, data

not shown). Also, PI staining followed by FACS analysis

showed that U937 and HL60 are both growth arrested after

PMA treatment (15ng/mL), see figure C. In constrast, KG-1

and KG-la did not show any difference in cell cycling. The

117

results obtained after PMA treatment were interesting

because KG-1 but not KG-la has previously been reported to

be PMA responsive, and KG-1 differentiates in response to

PMA treatment. Thus, the results show that after PMA

treatment of myeloid cell lines that lack aberrant pl5

methylation, pl5 is induced (HL60 and U937), but when

methylation is present pl5 (KG-1 and KG-la ), pl5 is not

induced. It still may simply be that KG-1 and KG-la are

lack responsiveness to PMA and a more direct experiment

would be homologous recombination of a methylated pl5 into

either HL60 or U937 to determine if this ablates PMA-

mediated pl5 induction.

118

1 2 3 4 5 6 7 8

pl5

8

Figure A. pl5 is induced by TGF-P in HaCaT, at the top is a Western blot for pl5, lanes: 1 = HaCaT, 2 = HaCaT +TGF-P, 3 = KG-1, 4 = KG-1 +TGF-P, 5 = KG-la, 6 = KG-la +TGF-p, 7 = U937, and 8 = U937 +TGF-P. Below is also shown Western blots for, from top to bottom, HL60, U937, KG-1, and KG-la. The lanes correspond to: 1 = HaCaT +TGF-p, 2 = untreated, 3-6=2, 4, 24, and 48 hour PMA treatment, 7 = 48 vehicle control treated, and 8 = pl5 protein.

119

HaCaT

+TGF-B *

vehicle

KG-la

vehicle KG-1

vehicle U937

vehicle

Figure B. Propidium iodide (PI) staining of cells followed by flow-assisted cytometry (FACS) after TGF-P treatment. As depicted with the asterisk (*), only HaCaT cells were growth arrested after TGF-P treatment.

120

61

vehicle

U937

+PMA*

vehicle

KG-I

vehicle

KG-la

vehicle

Figure C. Propidium iodide (PI) staining of cells followed by flow-assisted cytometry (FACS) after PMA treatment. As depicted with the asterisk (*), U937 and HL60 cells were growth arrested after PMA treatment.

121

APPENDIX B. SUMART OF D-BPLC AS A SZMPLB MSTBOD TO DSTXCT

ABBRRANT DNA MBTBTLATZCMf

We hypothesized that a cheaper and quicker method to

detect aberrant methyiation could be achieved by combining

sodium bisulfite modification and PGR amplification with

denaturing-high pressure liquid chromatography, D-HPLC. In

brief, we obtained sodium bisulfite modified DNA from U937,

KG-1, and KG-la. The 5' pl5 region then was amplified in

U937, KG-1, and KG-la by PGR. Figure A shows the

differences in the pl5 DNA methyiation patterns detected by

obtaining individual sequences of the cloned 5' pl5 sodium

bisulfite PGR products. In the 5' pl5 PGR product of

sodium bisulfite modified DNA there are ~10-12 base changes

in KG-1 and ~23 base changes in KG-la when compared to

U937. The PGR products were purified by ethanol

precipitation and quantitated with picogreen dye. The DNA

was then given to the D-HPLG core facility at the

University of Arizona. They ran 5 (iL of 15 ng/]xL of the pl5

sodium bisulfite modified PGR products from U937, KG-1, and

KG-la on a 55-70% 0.1 M triethylammonium acetate (TEAA) and

25% acetonitrile (AGN), 30-45% 0.1 M TEAA and 0.1% AGN,

gradient for 8 minutes at 58 degrees G on a DNAsep D-HPLG

column. The results obtained, shown in figure B, indicate

122

that D-HPLC is a valid method for distinguishing between

the three identified pl5 methylation states. The cost per

sample was $1.50. These results indicate that the use of

D-HPLC is a useful cheap and quick assay for determining

DNA methylation changes in any DNA sequence.

123

U937

100

80

60

:|La -MO -185

4u 120 -9

i i 49 113 182 297 367 436

KG-l

100

•440 -1*5 -120 "3 182 297 367 436

Figure A. The pl5 DNA methylation patterns segregates into unmethylated observed in U937, in blue, variegated methylation observed in KG-l, in red, and complete methylation observed in KG-la, in black. These three cell lines provide an ideal model to test whether D-HPLC can distinguish between the 5' pl5 PGR products of sodium bisulfite modified DNA.

124

I

I

r-r-f ̂ » 7 T

I I i i t I t < I i 1 I r-r

Figure C. Validation of concept: D-HPLC can distinguish between the 3 pl5 methylation patterns of U937, blue arrow, KG-1, red arrow, and KG-la, black arrow. The retention time of the KG-la PGR product is ~25 seconds greater than KG-1 and ~45 seconds greater than U937.

125

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