air filtration and radon decay product mitigation

17
Indoor Air, 2,84-100 (1992) 0 1992 Munksgoord, DK-Copenhagen Air Filtration and Radon Decay Product Mitigation C.S. Li and EK. Hopke2 Department of Chemistry, Clarkson University, Potsdam, NY 13699 Abstract Air cleaning as a means of mitigating the risks arising from ex- posure to indoor radon progeny has been evaluated in a single- family house in the north eastem US. using an auwmad, semi-continuous activipweighted size distribution measure- ment system. The measurements included radon concentration, condensation nuchi count, and activity-weighted size distribu- tion of radon decay products. Measurements were made in the house with and without an operating airjiltration system and with various particle sources common to normal indoor activi- ties operating. Aerosols were generated by running water in a shower, candle burning, cigarette smoking, vacuuming, opening doors, and cooking. Using a room model, the changes in attach- mmt rates, average attachment diameters, and deposition rates of the umttachedfraction with and without the air cleaning system were calculuted. In the presence of active aerosol sources, the air jiltration unit typtcally reduced the concentration of par- ricles within the hour follawng the end of particle generation. After candle burning, cigarette smoking, and vacuuming in the bedroom, the reductions of PAEC by airfilrration are about 60% with the airjiltration system operating in the bedroom. During cooking in the kitchen, the reductions of PAEC in the bedroom with the air jiltration system were about 40%. Hm- ever, for all cases the dose reductions were smaller than the par- ticle and PAEC reductions. For those particles that were gener- ated within the bedroom, there was a 20% to 50% reduction in dose. In the case of cooking where the dooT was open and parti- cles injiltrated from the rest of the house, the dose reduction was only 5% on average and appears to be insignificant. Thus, the dose reductions were h er than the reductions in activity con- centration, but there were no cases where the estimated dose ac- tually increased, KEY WORDS: Air filtration system, Radon decay products, Activity- weighted size distribution, Potential alpha energy concen- tration, Indoor aerosols, Radiation dose reduction. Manuscript received 10 June 1991 Accepted for publication: 9 April 1992 This paper contains parts of C.S. Li’s P b D . Thesis (University of Illinois. Urbana-Champaign). Current address: Department of Public Health, School of Medicine, National Taiwan University, Taipei, Taiwan. Author to whom correspondence should be directed. * Introduction The inhalation and lung deposition of the radon progeny produce adverse health effects. The U.S. Environmental Protection Agency estimated 20,000 deaths annually from radon-induced lung cancer (Puskin and Nelson, 1989). A dosimetric analysis of homes and mines has recently suggested that the dose in homes is slightly less than that to active un- derground miners (NRC/NAS, 1991) but the radon progeny still represent a significant health risk. It is thus necessary to control exposure to the radon progeny in order to lower the risk arising from in- door radon. Controlling radon progeny in the air space of houses may be divided into three principal categories: (1) preventing radon infiltration (base- ment pressurization, basement sealing, sub-slab de- pressurization, choice of building materials); (2) diluting the radon and radon progeny within the house (air-to-air heat exchanger, ventilation); and (3) using air cleaning systems for direct removal (fil- tration, mixing fan, electric field methods, radon ad- sorption, and ion generator). The use of various me- thods to reduce infiltration or to lower the concen- trations through increased ventilation have been under active study for several years. These systems can often be the most effective in reducing exposure, but until decisions have been made regarding the need for and nature of long-term solutions, interim measures for lowering exposure, e.g. air cleaning, are needed. Because of the studies of Rudnick et al. (1983) suggesting that air cleaning systems may in- crease risk in some situations, the EPA (1986) has not endorsed the use of air cleaners as a method of reducing radon decay products in indoor air. There have been a number of previous evalua- tions of air cleaning systems undertaken in test chambers or in actual indoor environments, and a review of these earlier studies has recently been compiled (Hopke et al., 1990). It demonstrated that air cleaning systems can effectively remove radon decay products from indoor air, although the reduc- tion of *18Po is not as great as that of 214Pb and *14Bi. At the same time, the particles are removed from the air. As a result, the unattached fiaction of air-

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Indoor Air, 2,84-100 (1992)

0 1992 Munksgoord, DK-Copenhagen

Air Filtration and Radon Decay Product Mitigation C.S. Li and EK. Hopke2 Department of Chemistry, Clarkson University, Potsdam, NY 13699

Abstract Air cleaning as a means of mitigating the risks arising from ex- posure to indoor radon progeny has been evaluated in a single- family house in the north eastem US. using an auwmad , semi-continuous activipweighted size distribution measure- ment system. The measurements included radon concentration, condensation nuchi count, and activity-weighted size distribu- tion of radon decay products. Measurements were made in the house with and without an operating airjiltration system and with various particle sources common to normal indoor activi- ties operating. Aerosols were generated by running water in a shower, candle burning, cigarette smoking, vacuuming, opening doors, and cooking. Using a room model, the changes in attach- mmt rates, average attachment diameters, and deposition rates of the umttachedfraction with and without the air cleaning system were calculuted. In the presence of active aerosol sources, the air jiltration unit typtcally reduced the concentration of par- ricles within the hour follawng the end of particle generation. After candle burning, cigarette smoking, and vacuuming in the bedroom, the reductions of PAEC by airfilrration are about 60% with the airjiltration system operating in the bedroom. During cooking in the kitchen, the reductions of PAEC in the bedroom with the air jiltration system were about 40%. H m - ever, for all cases the dose reductions were smaller than the par- ticle and PAEC reductions. For those particles that were gener- ated within the bedroom, there was a 20% to 50% reduction in dose. In the case of cooking where the dooT was open and parti- cles injiltrated from the rest of the house, the dose reduction was only 5% on average and appears to be insignificant. Thus, the dose reductions were h e r than the reductions in activity con- centration, but there were no cases where the estimated dose ac- tually increased,

KEY WORDS: Air filtration system, Radon decay products, Activity- weighted size distribution, Potential alpha energy concen- tration, Indoor aerosols, Radiation dose reduction.

Manuscript received 10 June 1991 Accepted for publication: 9 April 1992 ’ This paper contains parts of C.S. Li’s PbD. Thesis (University

of Illinois. Urbana-Champaign). Current address: Department of Public Health, School of Medicine, National Taiwan University, Taipei, Taiwan. Author to whom correspondence should be directed. *

Introduction The inhalation and lung deposition of the radon progeny produce adverse health effects. The U.S. Environmental Protection Agency estimated 20,000 deaths annually from radon-induced lung cancer (Puskin and Nelson, 1989). A dosimetric analysis of homes and mines has recently suggested that the dose in homes is slightly less than that to active un- derground miners (NRC/NAS, 1991) but the radon progeny still represent a significant health risk. It is thus necessary to control exposure to the radon progeny in order to lower the risk arising from in- door radon. Controlling radon progeny in the air space of houses may be divided into three principal categories: (1) preventing radon infiltration (base- ment pressurization, basement sealing, sub-slab de- pressurization, choice of building materials); (2) diluting the radon and radon progeny within the house (air-to-air heat exchanger, ventilation); and (3) using air cleaning systems for direct removal (fil- tration, mixing fan, electric field methods, radon ad- sorption, and ion generator). The use of various me- thods to reduce infiltration or to lower the concen- trations through increased ventilation have been under active study for several years. These systems can often be the most effective in reducing exposure, but until decisions have been made regarding the need for and nature of long-term solutions, interim measures for lowering exposure, e.g. air cleaning, are needed. Because of the studies of Rudnick et al. (1983) suggesting that air cleaning systems may in- crease risk in some situations, the EPA (1986) has not endorsed the use of air cleaners as a method of reducing radon decay products in indoor air.

There have been a number of previous evalua- tions of air cleaning systems undertaken in test chambers or in actual indoor environments, and a review of these earlier studies has recently been compiled (Hopke et al., 1990). It demonstrated that air cleaning systems can effectively remove radon decay products from indoor air, although the reduc- tion of *18Po is not as great as that of 214Pb and *14Bi. At the same time, the particles are removed from the air. As a result, the unattached fiaction of air-

Li and Hopke: Air Filtration and Radon Decay Product Mitigation 85

borne activity increases, especially for 218Po. Since the unattached fractions of the radon progeny are considered to be more effective in depositing their radiation dose to the lung tissue, concern has been expressed regarding the efficacy of air cleaning as a means of mitigating the hazards arising from indoor radon.

The main problem in the previous studies is that the systems used to measure the radon progeny were not able to determine their full size distribution, es- pecially in the range less than 10 nm. Estimates of the unattached fractions were made using measure- ment systems that provide a poorly defined size seg- regation (Ramamurthi and Hopke, 1989). In many cases, the progeny size measurement methods and results are not clearly stated. Therefore, further re- search is needed to measure the concentration and the size distribution of the radon progeny activities when air cleaning devices are employed.

In this study, the evaluations of an air filtration system were performed in a single-family house in Princeton, NJ. In a previous paper (Li and Hopke, 1991), we reported the influence of a series of particle generation processes on the exposure and dose re- sulting from the presence of the radon decay pro- ducts. In the study reported here, the same proce- dures are used to evaluate the effect of an air filtra- tion unit operating during the period when particles were actively being generated. The influence on the concentration and size distribution of radon progeny with and without the air cleaner in the presence of various active particle sources was evalu- ated. Using a simple room model (Jacobi, 1972; Por- stendorfer et al., 1978), the changes in various para- meters describing the behavior of the radon progeny were calculated for the conditions with and without the air filtration system, in the same manner as in the previous study (Li and Hopke, 1991). The dose to the cells of the bronchial epithelium were also calculated for each size distribution for two differ- ent breathing rates and for two different types of cells.

Air Filtration System The air filtration system used in this work was called a Pureflow Air Treatment System manufac- tured by the Amway Corporation, Ada, Michigan. It is a multi-stage filtering system containing a total of five separate filters: (1) a flexible, foam pre-filter which traps hair, lint, and large dust particles; (2&3) two activated carbon filters that contain two pounds

each of proprietary blends of a variety of specially treated activated carbons, supported uniformly in honeycomb beds, covered with white filter media and encased in a high quality aluminum frame; (4) a final carbon filter which is composed of activated carbon bonded to a non-woven substrate; and ( 5 ) a high efficiency particulate air (HEPA) filter that is designed to maximize filter efficiency, eliminate leaks and reduce the possibility of breakage. This HEPA filter contains the same filtering material used in many hospital surgical suite air filtration systems and industrial “clean rooms”. The pre-filter and activated carbon filters are installed at the back of the system. A third carbon filter and the HEPA filter are placed in front of the air filtration system. The air flows from the back to the front through the filters and the fan. The system’s microcomputer al- lows the programing of up to four different sets of ON-OFF times and fan speeds for automatic opera- tion. There are four fan speeds, 1.13, 2.26, 3.40, and 4.25 m3 mid . According to the manufacturer, the air filtration system gives maximum particle remo- val efficiency when operating at the highest speed (4.25 m-3 min-’). This highest speed was used for all of the experiments.

Measurement System for Radon Progeny Size Measurements The measurement system uses sampler/detector units incorporating wire screen and surface barrier detectors to determine the activity size distributions (Ramamurthi and Hopke, 1991). The use of this sys- tem for these measurements was described by Li and Hopke (1991). The PC-based analysis system al- lows the determination of the concentrations of 218Po, 214Pb and 214Bi (or 214P~) that penetrate to the filter in each sampler-detector unit using a spectro- scopy. Given knowledge of the penetration charac- teristics and the measured detection efficiency of each sampler, the activity size distributions can then be calculated from the observed activities and for the Potential Alpha Energy Concentration (PAEC) in six size intervals covering a particle size range of 0.5 to 500 nm (Ramamurthi and Hopke, 1991). The unattached fraction is defined in this study as the activity in the 0.5 to 1.6 nm region of the measured ac- tivity size distributions. These measured quantities and the uniformly mixed room model (Postendorfer et al., 1978) were used to estimate the values of para- meters relating to the rate of attachment of the radon progeny to the airborne particles, the deposition rate

86 Li and Hopke: Air Filtration and Radon Decay Product Mitigation

of that activity that remained uncombined with the particles, and the average size of the particles to which the activity had become attached. The details of these calculations are given by Porstendorfer (1984), Reineking et al. (1985), and Porstendorfer et al. (1987). The size dependent rates for the attach- ment for the radon progeny to particles was taken from Porstendorfer et al. (1979).

Dosimetric Calculations The alpha radiation dose to the bronchial epitheli- um has been calculated using the model developed for the recent report of the National Research Coun- cil (1991). In this model, the average dose (mGy) per unit exposure to PAEC (in WL) has been calculated for both basal and secretory cells of generations 0 to 8 of the tracheobronchial tree at several breathing rates. A plot of dose conversion coefficients as a function of particle size, cell type, and breathing rate were given by Li and Hopke (1991). The lower breathing rate for each cell is 0.45 m3hr-' (Bl, Sl), while the highest likely breathing rate (Bh, S,) is 1.5 m3hr-'.

The hourly dose rate per Bq m-3 radon can be es- timated from these dose conversion coeficients and the measured size distributions as follows. The PAEC in each size range can be obtained from the measured total PAEC and the PAEC fractional size distribution. The PAEC in each size interval is mul- tiplied by the dose conversion factor determined at the mid-point of every size interval, providing esti- mates of the dose in every size interval. Summing these doses over all six size intervals and dividing by 170 hours (a working month) and the radon concen- tration, the hourly dose rate per Bq m-3 radon can be calculated.

Results of Field Sampling in Princeton, NJ The measurements were made in collaboration with the Center for Energy and Environmental Studies (CEES) at Princeton University. Houses have been identified and instrumented for continuous meas- urement of radon and physical parameters including basement, bedroom, and subslab radon concentra- tions, pressure differences across the basemendout- side south interfaces, basemendsubslab, basemend upstairs, and basemendoutside east interface, tem- peratures in basement, upstairs, outside, and soil. House 21 was a one-story residence with a living

room, a dining room, a kitchen, two bedrooms, a study, two bathrooms, and a basement. A floor plan for this house was given by Li and Hopke (1991). Activity size distributions were also measured in the living room and the master bedroom over a two- week period. A total of about 10 measurements were made in the living room and more than 100 meas- urements in the bedroom. The particle concentra- tions were measured by using a Gardner manual condensation nucleus counter. This device has an ef- fective minimum detection limit of 1000 ~ m - ~ . The concentration and size distribution of radon progeny were determined using a 75-minute total interval to maximize the number of distributions measured on the evolving aerosol.

The evaluation of the air filtration system was made by operating different types of particle gener- ation with and without the air cleaner operating. Particles were generated by running a shower, burn- ing a candle, allowing a cigarette to smolder in an ashtray, vacuuming (electric motor), opening the room door, and cooking. In each case, the particles were generated for a period of 20 minutes. Five minutes into the particle generation period, a 15- minute sampling interval with alpha counting was initiated so that the particle generation and the Sam- ple intervals terminated at the same time. After a 20-minute decay time, a second count of 40 minutes was obtained before starting the next sampling/ counting cycle. A third sample was obtained begin- ning at 135 minutes after the end of the particle gen- eration period so that the evolution of the airborne activity over time could be evaluated. Two separate experiments were performed for each particle gener- ation activity. The activity size distributions pro- duced by these various aerosol sources when the air cleaner was not operating and the resulting calcula- ted bronchial dose have been represented by Li and Hopke (1991).

Background Conditions Door Closed The air cleaning studies were performed in the mas- ter bedroom which adjoined one of the bathrooms. The infiltration rate had been measured by CEES group to be around 0.3 hr-l with the interior doors open and all the windows in the house closed. Therefore, the ventilation rate was assumed to be 0.2 hr-' with the bedroom door closed. Figure 1 shows the average size distribution obtained from three activity size distributions measured for each of the radon progeny and PAEC under background

Li and Hopke: Air Filtration and Radon Decay Product Mitigation 87

conditions of the bedroom door shut and after the air filtration system had been running for at least 2 hours. The results of the measurements, room model, and dosimeuic model calculations are pres- ented in Table 1. This table presents the measured 222Rn concentration (Bq m-3), C,,, the measured con- densation nuclei concentration (lo3 ~ m - ~ ) , Z, the un- attached fraction of 218Po, f,, the unattached fraction of PAEC, f,, and the equilibrium factor, E Calcula- ted values are the average attachment rate, X, the at-

tachment average diameter, d, the deposition rate for the unattached progeny, q("), and the dose to basal and secretory cells at low (1) and high (h) breathing rates.

With the bedroom door closed and the air filtra- tion system off, the background conditions of the bedroom are: (1) the particle concentration was about 2,500 to 3,000 ~ m - ~ ; (2) the unattached frac- tion of 218Po was between 0.5 and 0.7; (3) the unat- tached fraction of PAEC was between 0.2 and 0.4;

Table 1 Measurement, room, and dose model results for the closed door experiments with the air cleaner operating.

G Z fi fP (Bq/m3) (l W C ~ - ~ )

Dose (~Gyhr-'/Bqrn-~) Basal (1, h) Secretory(1, h)

477 1.8 0.931 0.500 (cleaner on for 4.0 hours) 382 1.8 0.933 0.621 (cleaner on for 5.5 hours) 429 1 .o 0.967 0.835 (cleaner on for 4.0 hours) 444 1 .o 0.967 0.825 (cleaner on for 6.0 hours) 408 1 .o 0.934 0.754 (cleaner on for 8.0 hours) 777 1 .o 0.933 0.681 (cleaner running for 4 hours, background) 323 1.8 0.967 0.801 (cleaner on for 6 hours) 300 1.8 0.967 0.777 (cleaner on for 7.5 hours) 302 1 .o 0.934 0.712 (cleaner on overnight) 520 1 .o 1.000 0.841 (cleaner on for 0.4 hours) 41 6 1.8 0.967 0.803 (cleaner on for 4.0 hours)

0.14 18.1

0.164 16.9

0.1 36 15.7

0.132 15.8

0.1 34 14.8

0.163 34.2

0.158 13.8

0.164 13.3

0.103 8.4

0.113 15.9

0.147 16.5

1 .o

1 .o

0.46

0.46

0.96

0.97

0.40

0.40

0.96

0.00

0.46

30

30

26

26

36

36

18

20

36

10

19

19

11

7.5

9.99

11.9

7.6

9.4

8.9

16.6

12.9

8.5

3.5,10.6

3.9,13.1

3.9,13.8

3.7,13.3

3.7,12.7

4.1,14.1

4.5,15,7

4.4,15.7

2.8,9.6

3.2J1.5

4.8,15.7

7.5,23.2

8.5,28.6

8.6,30.5

8.3,29.3

8.0,27.9

9.0,31 .O

9.8,34.4

9.8,34.5

6.2,21.1

7.1,25.4

10.4,34.3

1 .o

0.0 1 10 100

Particle Diameter (nm) Fig. 1 Average activity size distributions meas- ured in the bedroom with the closed door and the air filtration system operating.

88 Li and Hopke: Air Filtration and Radon Decay Product Mitigation

0-

E d

(4) the equilibrium factor was in the range of 0.3 to 0.5; (5 ) the attachment rate was between 6 and 14 hr-l; (6) the average attachment diameter was about 50 to 90 nm; and (7) the deposition rate of the unat- tached fraction was around 4 to 12 hrl. With the air fil- tration operating, more than 95% of 21aPo was in the 0.5 to 1.6 nm size range. The fractions of *14Pb and 214Bi in the 0.9 nm size range were about 80% and 50%, re spectively These results showed that the air filtration system effectively removed most of the particles in the bedroom. There was an insignificant fraction of the three distributions in the 1.6 to 16 nm size range. The values of PAEC and dose per unit radon are shown in Figure 2. The average PAEC reduction was about 60% while the reduction in dose was 31%.

Bedroom Door Open When the bedroom door was open and the air filtra- tion system operating, the particle concentration was reduced to 6,000-7,000 cmd from approximate- ly 10,000 ~ m - ~ . Average activity size distributions for a series of measurements are shown in Figure 3. The unattached fraction of 218 Po was still high (90%), but slightly lower than when the bedroom door was closed and the air filtration system operating. This result is due to the higher ventilation rate under these conditions. Particles continued to enter the bedroom as the air filtration system created addi- tional air circulation. Thus, radon decay products became attached to particles with the bedroom door open. The unattached fraction of 218Po and PAEC were between 0.87 and 0.93 and ranged from 0.58 to 0.63, respectively. The fraction of 214Pb and 214Bi in the 0.9 nm size range was about 25% and 18%, re- spectively. No 218Po activity was observed in the 1.5- 5 nm size range but 30% of the 214Pb and 214Bi was observed. The results of the measurements, room model, and dosimetric model calculations are shown in Table 2.

Since there were no active particle sources operat- ing, it is assumed that the particles in this size range were probably the result of leakage from the oil-fired forced air furnace. The emittance of particles of a si- milar size had previously been observed fiom a leak- ing furnace in a house in Springfield, PA (Li, 1990). These particles were observed in a number of the measured size distributions. The variation in the particle concentration and size distributions that oc- curs when the door is open is presumed to be re- sponsible for the much greater variability in the measured and inferred quantities. In summary, a bi- modal size distribution was observed for all three

v Cleaner O n 8 Cleaner Off

20

'g

v 9 IS:

8

'$ I I

I . , . , . , . , . . v Cleaner On . Cleaner Off

8 8 '

I 8 I - . . . - - 8 .

v

O . O l . ' . ' . ' ' " * . I 0 2 4 6 8 10 12

Sample Number

Sample Number

Fig. 2 Top: PAEC per unit radon for the series of samples taken in the bedroom with the door closed.

Bottom: Dose per unit radon concentration for the series of samples taken in the bedroom with the door closed.

1 .o

0 Po-218 v Pb-214 - Bi-214

PAEC

1 10 100

Particle Diameter (nm)

Fig. 3 Average activity size distributions measured in the bed- room with the door open and the air filtration system operating.

Li and Hopke: Air Filtration and Radon Decay Product Mitigation 89

0.2

0.1

0.0

Table 2 Measurement, room, and dose model results for the open door experiments with the air cleaner operating.

G Z fi f* F PAEC X d q(U' Dose (pGyhr1/Bqm'3) (Bq/m3) (103cm-3) (mWL) (hr') (nm) (hr') Basal (1, h) Secretory& h) 870 7.0 0.833 0.323 0.370 76.0 2.1 21 6.0 9.0,26.2 19.7,57.3

1544 6.0 0.828 0.416 0.235 98.0 1 .o 17 9.2 7.0,20.5 15.2,44.9

994 6.0 0.897 0.415 0.227 61 .O 1.5 19 7.7 7.1,20.9 15.6,45.7

713 6.0 0.897 0.473 0.228 44.0 1.5 19 8.8 7.0,21.0 15.3,46.0

436 8.0 0.678 0.321 0.189 22.3 5.9 33 29.3 4.4,11.6 9.3,25.0

472 8.0 0.722 0.331 0.216 27.6 4.8 31 19.5 5.2,13.9 11.1,29.9

513 7.5 0.707 0.309 0.201 27.9 5.3 33 28.0 4.4,11.7 9.4,25.2

(cleaner on for 6.0 hours)

(cleaner on for 2.0 hours)

(cleaner on for 3.5 hours)

(cleaner on for 7.0 hours)

(cleaner on for 2.0 hours)

(Cleaner on for 3.5 hours)

(cleaner on for 7.0 hours)

. , . , . , . , . , . i

v Cleaner On Cleaner Off

= I

b m v = m

----Ft" --_--_-I -------------- 7 r T

, . , . I .

T Cleaner O n Cleaner Off

0 2 4 0 8 10 12

Sample Number

Fig. 4 Top: PAEC per unit radon for the series of somples taken in the bedroom with the door open.

Bottom: Dose per unit radon concentration for the series of samples taken in the bedroom with the door open.

decay products with a major mode (80%) in the 0.5- 5 nm size range and a minor mode (20%) in the 50- 500 nm size range. The equilibrium factor decreased from 0.50 to 0.23. A decrease in the attachment rate (from 4 hr-' to 2 hr-') and average attachment dia- meter (from 30 nm to 24 nm) was observed com- pared with the background conditions without the air filtration system. The deposition rate of the un- attached fraction increased from 3 hr-' to 7 hr-'. The values of PAEC and dose per unit radon are shown in Figure 4. The reduction in PAEC per Bq m-3 ra- don was 39% and the dose reduction was 31% com- pared to the condition without the air filtration sys- tem.

Candle Burning To examine the influence of an open flame on the radon progeny concentrations and size distributions as well as the effectiveness of the filtration system to remove these particles, a single candle was burned in the closed bedroom. The effect on the radon progeny behavior of the filtration unit operation during and after the candle burning is shown in Figure 5. The results of duplicate experiments are presented. These results can be compared with those measured without the air cleaner operating (Li and Hopke, 1991). The fraction of 218Po changed from 95% to 65% in the 0.9 nm size range during candle burning, then back to 95% after 65 minutes. The fraction of 214Pb in the 0.9 nm size range is about 70% (background, 60 minutes later, and 135 minutes later) and 50% during candle burning. During can- dle burning, there is a 10% fraction of 218Po in the 1.5 to 5 nm size range, but an insignificant fraction in the background 60 minutes later, and 135 minutes

90 Li and Hopke: Air Filtration and Radon Decay Product Mitigation

0.8

4 8 .-

0.6

C

3 u d

Rn = 295 Bq XI-'

CN Conc. = 2.000 cm-'

0 *lSPo = 202 Bq rn

!&a

0.8

g 0 el4 Pb = 43 Bq m-' (5.3%) 3

0 Et:

-3 .

(3.02)

114 3 0.6 - A Bi = 49 Bq m-' (6.4%)

Rn - 368 Bq m-' CN Conc. - 80.0oo cp-' 0 *"Po - 25s Bq m-' (2.7%)

Pb - 60.7 Bq tn-' (5.0%) Bi = 40.0 Bq m-' (8.8%)

0.8

o PIEC - 18.1 mWL (1.2%) 0.6

k A PAEC = 16.5 mWL (1.2%) h 4 '6 0.4 ~

3 8

0.2 :=a - -

r . I I . . .~ 0.0 - ' ' . "'

c 0.4 1 .I 4

2

A 5 0.4 3 8

0.2

0.0

1 10 100

Particle Diameter (nm)

During candle burning interval (first experiment).

1 .o

0.8

E E 3

Ir A 5 0.4 3 4

0.6

0.2

0.0

u t Rn = 320 Bq m-' '

CN ~onc. = 2.000 cm-' 0 "'Po = 188 Bq m-' (3.1%) A "'Pb = 45.5 Bq m-' (&EX) A Bi - 38.6 Bq m-* ( 7 3 2 ) D PAEC = 15.3 mVL (1.2%)

LZL

114

\

- . . 1 ..- r . . . . , I . . . 1

- 10 100

Particle Diameter (nm)

60 minutes after the bum interval.

1 .o 414 B q m-'

CN Conc. = so.O0O crn-' 0 ""Po - 272 Bq =-* (2.6%)

3 3 L. 0.6 31 Eq m-' (11.0%) k4

h 4 3 0.4

4 4

0.2

0.0 1 10 100

Particle Diameter (nm)

During candle burning interval (second experiment).

1.0 , . . . . , 0.8

A 0.6 1 5 0.4 3 0 *

0.2

0.0 1

334 Bq m-' CN conc. = 1,000 cm-'

921 Rn=

0 ""Po = 264 Bq m-' (2.6%) 0 ' lbb L14 = 48 Rq m-' (5.42) A Bi = 36 Bq m-' (10.1%) A PAEC = 18 mwL (1.2%)

10 100

Particle Diameter (nm)

60 minutes after the bum interval.

1.0, . 1 I 1 .o I ' . . . ' I

F a = 41 ~q m-' 222

CN Conc. = 1,000 cm-'

0 ""Po = 284 Bq m-' (2.6%) 0 *14Pb = 56 Bq rn-' (432) A Bi = 42 Bq m-' (8.9%) A PAEC = 20 mWL (1.1%)

L14

1 10 100

Particle Diameter (nm) Particle Diameter (nm)

130 minutes after the burn interval. 130 minutes after the bum interval. Fig. 5 Activity size distributions measured when particles were generated by a burning candle with the air filtration system operating.

Li and Hopke: Air Filtration and Radon Decay Product Mitigation 91

Table 3 Measurement, room, ond dose model results for the candle burning experiments with the air cleaner operating.

6 Z fi fP F PAEC X d p Dose (~Gyhr-'/Bqm'~) (Bq/m3) (1 03cm-3) (mWL) (hr-I) (nm) ( h r - I ) Basal (1, h) Secretory(1, h)

( I ) 359 80 0.667 0.500 0.187 18.1 4 10 7 5.3, 15.6 1 1.5,34.1 (during candle burning, cleaner on for 7 hours)

(55 minutes after candle extinguished)

(1 30 minutes after candle extinguished)

(205 minutes after candle extinguished) (*I414 60.0 0.667 0.507 0.165 18.4 5.82 15 9.86 4.3,13.2 9.5,28.8 (cleaner on for 10 hours, during candle burning)

(55 minutes after candle extinguished)

( 1 30 minutes after candle extinguished)

320 2.0 0.931 0.655 0.1 77 15.3 1 26 10 4.4, 14.8 9.5,32.4

295 2.0 0.931 0.552 0.207 16.5 1 26 7 5.4,16.9 11.8,36.9

316 2.0 0.933 0.633 0.190 16.2 0.9 24 7 4.9,16.4 10.8, 35.9

334 1.0 0.936 0.768 0.194 17.5 0.93 35 3.77 5.2,18.4 11.5,40.5

446 1 .O 0.934 0.726 0.163 19.7 0.96 36 8.16 4.2,14.8 9.3, 32.4

later. Very few of the three distributions are in the 5 to 15 nm size range. The results of the measure- ments, the room and dose models are given in Table 3.

With the air filtration system operating, the effect of radon decay products from candle burning are: (1) the unattached fraction of *lSPo and PAEC decreased from 0.93 to 0.73 and from 0.76 to 0.57; (2) the equi- librium factor increased from 0.14 to 0.18; (3) the at- tachment rate increased from 1 hr-' to 4 hr-' during candle burning (from 1,800 ~ m - ~ to 60,000 ~ m - ~ ) , to 1 hr-I afier 60,135 minutes (1,500 ~ m - ~ ) ; (4) the aver- age diameter changed from 30 nm to 13 nm during candle burning, to 30 nm after 60 minutes; and (5) the deposition rate of the unattached fraction de- creased from ll hr-l to 9 hr-' during candle burning. The CN counts for each of the two experiments are shown in Figure 6. The particle concentration in- creased during particle generation activity and then declined more rapidly than observed in the absence

h lo8 0 1 0 0 Jan 23, 1990 1

1990

e-- I 75

Time (minutes)

Fig. 6 CN counts as a function of time during the candle burn- ing experiments with the air filter operating.

v Cleaner On m Cleaner Off

0 1 2

Time (hours)

Fig. 7 Top: PAEC per unit radon concentration 0 s o function of time from the start of the sample token while the candle was burning.

time from the stort of the somple token while the candle was burning.

Bottom: Dose per unit radon concentration 0 s o function of

92 Li and Hopke: Air Filtration and Radon Decay Produd Mitigation

1.0

0.8

3 5 0.6 h h $ 0.4

3 2 0.6

x 5 0.4 3

A PABC = 17.0 m a (1.1%)

Y 0.2

. . .,

.p Rn = 641 Bq m-' CN Conc. = 30.006 em-'

- 0 "'Po - 670 Bq ma (1.8%) 0 '"Pb = - Bi = 56 Bq mJ (10.4%)

104 Bq m-' (2.3%) ., X I 4

A Puc 51 mWL (0.7%)

0.0

1.0

0.8

.I 4

0 0.6 k h 5 0.4

Part icle Diameter (nm)

....,

222 Rn = 625 Bq m-' - CN Conc. = 1.800 Em-'

0 "*Po = 360 Bq m-a (2.3%)

- A a14 BI = 71 Bq rn-' (8.0%) 0 *14Pb - 110 Bq m-' (2.9%) '

A PAEC = 33 mllz (0.8%) . - 0

1.0

0.8

5

2

.I 4

2 0.6

3 Y

10 100 1

, . . . - , ctp Rn = 192 Bq m-'

CN Conc. = 1,800 cm-'

0 "'Po = 121 Bq m-' (2.5%) 814 Pb = 38 Bq rn-' (3.0%) 214

A Bi = 21 Bq m-' (5.8%) A PAEC = 10.8 m l z (1.0%)

.

Part icle Diameter (nm)

During the cigarette smoldering interval (first experiment) experiment)

During the cigarette .smoldering interval (second

Rn = 204 Bq m-' CN Conc. = 1.800 cm

0 ''*PO = 115 Bq m-' (2.6%)

"'Pb = 34 Bq m-' (3.3%) 81 = 27 Bq m-' (4.4%)

c 0

2 0.6

x

." 0

A PAEC = 10.8 mWL (1.OX)

4

k

f :::I, 4 A-A

100

0.0 /- 1 10

Part icle Diameter (nm)

60 minutes after the burn interval 60 minutes after the bum interval

135 minutes after the bum interval Fig. 8 Activity size distributions measured when particles were generated by a cigarette smoldering with the air filtration system operating.

Li and Hopke: Air Filtration and Radon Decay Product Mitigation 93

Table 4 Measurement, room, and dose model results for the cigarette burning experiments with the air cleaner operating.

GI Z fi fP F PAEC X d q'"' Dose (pG~hr-'/Bqm-~) (Bq/m3) (103cm3) (mWL) (hr') (nm) (hr-') Basal (1, h) Secretory(1, h)

('1 207 50 0.097 0.167 0.304 17.0 92 52 8 5.7,11.6 11.9,24.4 (cleaner on for 4 hours, during cigarette smoking)

204 1.8 0.774 0.467 0.193 10.6 4 60 13 4.7,14.0 10.1,30.6 (after 60 minutes)

192 1 .8 0.800 0.448 0.208 10.8 3 50 10 5.0,14.9 10.8,32.2 (after 135 minutes) (2)641 30.0 0.067 0.115 0.295 51.1 122 85 12.5 4.9,ll.O 10.3,23.3 (cleaner on for 5.5 hours, during cigarette smoking)

625 1.8 0.767 0.435 0.192 32.5 4.12 61 12.1 4.4,13.4 9.6,29.2 (after 60 minutes)

of the operating air filter (Li and Hopke, 1991). The PAEC and dose to secretory cells at a breathing rate of 0.45 m3 hr-I per unit radon are shown in Figure 7. The lines are drawn through the points only to sug- gest the trends in the results. With the air filtration system, the PAEC decreased 53% from the value ob- served with the candle burning alone. The dose re- duction averaged over the duplicate set of 3 meas- urements was 28%.

Cigarette Smoldering A cigarette was allowed to burn in an ashtray produ- cing only sidestream smoke in the closed room. For the measurements without the air cleaner (Li and Hopke, 1991), the fraction of 21*Po in the 0.5 to 1.6 nm size range changed fiom 67% to 8%. The frac- tion of 214Pb and 214Bi in this smallest size range was about 10% before the cigarette was lit and showed a significant reduction to essentially zero so that the unattached fraction of PAEC declined to 7% from an initial value of 31%. The fraction of three distri- butions in the 1.5 to 15 nm size range remained the same. A large increase in the 50 to 500 nm size

h lo8 . . . . , . . - . . . . . 0 I

0 Jan 24. 1990

I 0 JM 28. 1900 {

4 0-0-0 ' 0 -

10% I 0 25 50 75 100

Time (minutes)

Fig. 9 CN counts as a function of time during the cigarette burn- ing experiments with the air filter operating.

0.2 , I

2 s w 4 a

0 1 2

Time (hours)

Cleaner Off n

I 1 2 3

Time (hours)

Fig. 10 Top: PAEC per unit radon concentration as a function of time from the start of the sample taken while the cigarette was smoldering.

Bottom: Dose per unit radon concentration as a function of time from the start of the sample taken while the cigarette was smoldering.

94 Li and Hopke: Air Filtration and Radon Decay Product Mitigation

range was observed for 218Po (from 40% to 80%) with only small changes for 214Pb and 214Bi (from 35% to 40%). Without the filtration system operating, the particle concentration increased significantly (up to 100,000 ~ m - ~ ) during burn interval, then declined to a steady-state concentration of around 8,000 ~ m - ~ . Thus, without the air cleaner, the cigarette smoke particles remain for an extended period of time and substantially perturb the activity-weighted size dis- tributions.

With the air cleaner operating, the size distribu- tions measured in the cigarette smoke experiments are shown in Figure 8. The fraction of 218Po changed from 95% to 10% in the smallest size range after 5 minutes, then increased back to 80% in the later dis- tributions. The fraction of 214Pb and 214Bi in the 1.6 to 5.0 nm range was 8% after 5 minutes, but re- turned to 25% by the 60-minute measurement. Very little activity appears in the 1.6 to 15 nm size range for samples at 60 or 135 minutes, but 15% was present at 5 minutes. The results of the measure- ment, the room and dose models are given in Table 4.

The attached mode activity increased from 20% to 80% in the sample obtained during the particle generation interval, then returned to the back- ground condition by the second measurement. The air filtration system thus rapidly removed the parti- cles from the air as shown in Figure 9. The changes in PAEC and dose over time are shown in Figure 10. The average decrease in PAEC per unit radon was 56% compared to the case where the filtration unit was not functioning, but a reduction in dose per unit radon occurred only during the period begin- ning 60 minutes from the end of the particle gener- ation interval, although the average reduction was 24%.

Vacuuming With the door closed, a portion of the carpet was va- cuumed for 20 minutes to produce particles smaller than 100 nm, similar to those produced fiom candle burning. These results were similar to those ob- served by Reineking and Porstendorfer (1986). They found an additional mode in the size range 20 to 80 nm formed by the particles generated from an elec- tric motor. In the first experiment with the air clea- ner off, the particle number concentration reached 90,000 ~ m - ~ , then decreased to 4,000 ~ m - ~ at 135 min- utes after the end of vacuuming. A significant addi- tional mode in 218Po activity distribution was found in the 15 to 100 nm size range because of the attach- ment of 218Po to the small particles produced by the motor (Li and Hopke, 1991).

However, in the second vacuuming experiment, a significantly smaller concentration was observed (15,000 cm-’) during the particle generation period. The lower concentration caused a variation in the size distribution of radon decay products. A moder- ate activity decrease in the 0.9 nm size range was ob- served for 218Po (about 40%) and a smaller result for z14Pb and 214Bi (about 10%). The unattached fraction of z18Po decreased during the particle generation to 35%, and increased back to 56% at 60 minutes after the end of vacuuming, and finally to 67% at 135 minutes after the end of vacuuming. The unattached fraction of PAEC decreased from 45% to 16% during the particle generation period, and returned to 30% in the sample taken 60 minutes after the end of va- cuuming. The equilibrium factor increased from 0.24 to 0.26 (during the particle generation period), to 0.34 (60 minutes after the end of vacuuming), and to 0.28 (135 minutes after vacuuming stopped). The average attachment diameter of these small particles was smaller, and thus, a lower attachment rate was

Table 5 Measurement, room, and dose model results for the vacuuming experiments with the air cleaner operating.

F PAEC X d q(U’ Dose (~Gyhr-’/Bqm”) (Bq/m3) (103cm-3) (mWL) (hr-‘) (nm) (hr-I) Basal (1, h) Secretory(1, h) 6 2 fi fP

(l) 179 40 0.667 0.487 0.126 6.1 3.4 12 13.7 4.1,12.0 9.0,26.3 (cleaner on for 9.5 hours, during the vacuuming)

118 1.8 0.937 0.754 0.1 15 3.7 0.9 26 12.1 3.1,10.9 6.8,23.9 (after 60 minutes)

72 1.5 0.967 0.700 0.124 2.4 0.5 22 11 3.6,12.0 8.0,26.4 (after 135 minutes)

285 18 0724 0.554 0.131 10.1 3.54 17 12.7 4.0,12.0 8.8,26.3 (during the vacuuming)

(after 60 minutes)

(after 135 minutes)

303 1 0.934 0.711 0.170 13.9 0.95 36 7.5 4.6,15.7 10.2,34.4

328 1 0.967 0.735 0.160 14.2 0.46 26 7.9 4.3,14.9 9.4, 32.7

Li and Hopke: Air Filtration and Radon Decay Product Mitigation 95

1.0 . . . L 1 . 0 - - - . - . 1 Rn = 328 Bq m-'

CN Conc. = 1.000 cm-'

PP Rn = 72 Bq m-3 pep

0.8 . CN cone. = 1.500 Em-' 0.8 .

E 0 21ePo = 40 Bq m-' (6.3%) E a 0 2c8Po = 208 Bq m-' (2.9%) 0 o 214 Pb = 6 Bq m-'(17.7%) 4 o Pb = 40 B q m-3 (5.7X)

2 0.6 . A Bi = 29 Bq m-' (lO.9Z) - A Bi = 5 Bq m-' (27.1X) A PAEC = 2.1 mWL (3.5%) 2. A PAEC 14 mWL (1.4%) .

h -s 0.4 .

<

214

214

._ 214

4

.- 4

0.2 . /A - 0.0 . _ _ _ ' ' I \.-* m :

1 .o

0.8

3

k 3 V m 0.6

A '5 0.4

<

+I

.- z

0.2

0.0

I .

Rn = 178 B q m-' Po1

CN Conc. = 40 .W cm-"

0 '"Po - 9&l Bq m-' (4.1%)

0 '"Pb = 16 Bq m-' (10.1%) A Bi = 13 B q m-' (17.4%) A PAEC = 6.1 mWL (2.2%)

214 Tl ,,,J A A A

1 10 100

Particle Diameter (nm)

During the vacuuming period (first experiment ).

1.0,. . . I

991 Rn = 118 Bq m-' CN Conc. = 1.~00 cm-3

0 21aPo = 64 Bq m-' (5.1%) t14

X I 4 Pb = 10 Bq m-' (ll.E%)

A Bi = 5 Bq m-' (37.2%) A PAEC = 3.7 mWL (2.9%)

1 10 100

Particle Diameter (nm)

60 minutes after vacuuming.

1.0 . . . . .

0.8

5 3 V

r4 0.6

R 2 0.4 3 4

0.2

0 4 = 285 Bq m-'

CN ant. = 18,000 cm4

0 2'"Po - 162 Bq m-$ (3.3%) ¶I4 Pb = 90 Bq m-' (6.6%)

A PAEC = 10 mWL (1.7%)

A 214 Bi = 16 Bq m4 (19.0%)

0.0 '

1 10 100

Particle Diameter (nm)

During the vacuuming period(second experiment).

1 .o

0.8 c 4 V 6 0.6

.d

r2

4

x 3 0.4 .- +I

0.2

0.0

-

0

\ 1

"Rn = 303 Bg m-a CN Conc. = 1.000 cm-'

0 ""Po = 198 Bq m-' (3.0%)

Pb = 45 Bq m-3 (4.5%) A Bi = 22 Bq m-' (14.0%)

214

9.14

A PAEC I 14 mWL (1.4%)

I . . . . t I . . 10 100

Particle Diameter (nm)

60 minutes after vacuuming.

Particle Diameter (nm)

135 minutes after vacuuming.

Particle Diameter (nm)

Fig. 11 Activity size distributions measured when particles were generated by vacuuming in the room with the air filtration system oper- ating.

96 Li and Hapke: Air Filtration and Radon Decay Product Mitigation

observed (50 hr-I). The activity-weighted size distri- butions returned to those of the background con- dition gradually after vacuuming was discontinued. The deposition rate of the unattached fraction in- creased from 5 hr-' to 30 hr-'.

The results of the duplicate experiments with the air filter operating are presented in Figure 11 in the form of the activity-weighted size distributions. The results of these measurements, the room, and dose models are given in Table 5. The CN counts as a function of time are shown in Figure 12. The first experiment appears to follow the expected pattern, but in the other experiment on January 29, the CN count declined much more slowly than would have been expected. The reason for this discrepancy is unknown. The PAEC and dose per unit radon for the experiments with and without the air cleaner running are shown in Figure 13. The activity in the smallest size range was observed to be 70% for 218Po, and 30% for 214Pb and 'I4Bi. The unattached fraction of *'To decreased from 0.93 to 0.80. The unattached fraction of PAEC decreased from 0.74 to 0.62. The equilibrium factor changed insignificantly. A mod- erate decrease in the unattached fraction during the vacuuming period was observed both with and with- out the air filtration system. A 25% increase in the 1.5 to 50 nm size range was observed for 218Po due to the attachment of decay products to the small parti- cles generated from vacuuming. A 30% increase in the 1.5 to 150 nm size range was also observed for all three size distributions. The size distributions of the 60 and 130 minute measurements were very similar to the background condition. The attachment rate increased from 1 hr-* to 3.5 hrl during the active par- ticle period, and decreased to 0.8 hr-' after 60 and 135 minutes. The average diameter decreased from 30 nm to 15 nm during the active particle period, and to 26 nm after 60 and 135 minutes. The average reduction in PAEC per Bq m-3 radon was 60% and the average dose reduction was 49%.

Cooking A steak was pan fried for 20 minutes using the gas stove in the kitchen. The bedroom door was open for these experiments. During the cooking experi- ment with the air filtration system 0% the particle number concentrations were found to be 250,000 ~ m - ~ in the kitchen and 30,000 ~ m - ~ in the bedroom. With the air cleaner off, only 10% activity of all three size distributions was in the 0.9 nm size range. The unattached fraction of PAEC was 0.15 with the equi- librium factor of 0.50. All three size distributions in

' E 0 Jan 25, lQ90

0 Jan 28. l9QO 0

c

a L.l 4

v

$ to'

8 2 104

0

u a 0 d

a 10' 0 25 50 75

Time (minu tes)

Fig. 12 CN counts as a function of time during the vacuum clea- ner operation with the air filter operating.

m Cleaner Off

m

0 I a 3

Time (hours)

f

1 0 1 t S

Time (hours)

Fig. 13 Top: PAEC per unit radon concentration as a function of time from the start of the sample taken while the vacuum clea- ner was operating.

Bottom: Dose per unit radon concentration as a function of time from the start of the sample taken while the vacuum clea- ner was operating.

Li and Hopke: Air Filtration and Radon Decay Product Mitigotion 97

the bedroom were bimodal, with a major mode in the attached size range (80%). A significant increase in the attached fraction larger than 20 nm was ob- served in the bedroom. The average attachment dia- meter increased from 25 to 50 nm during the par- ticle generation period, and to 80 nm at 60 and 135 minutes after the end of the cooking interval. Rein- eking et al. (1985) reported a 74 nm attachment dia- meter for particles produced from a tiled stove and cooking aerosols. Tu and Knutson (1988) measured the particle size distributions in two homes. They found that the size ranges were different for cooking soup and frying meat and eggs. The soup particles produced using a gas stove are smaller in size, with a mean diameter of 14 nm. Particles from frying food had a mean diameter of 54 nm. Tu and Knutson’s results are in general agreement with the activity size distributions obtained in the bedroom after fiy- ing a steak in the kitchen.

The larger particles observed in the bedroom from cooking had higher attachment rates than the smoldering cigarette particles. The attachment rate increased from 6 hr-’ to 40 hr-’ during the particle generation period, and to 48 hr-‘ after 60 and 135 minute samples. It appears that the particles took a moderate time moving from the kitchen to the bed- room. The size distributions of three decay products remained the same for longer periods of time.

Strong (1988) found a quite different size distribu- tion of radon decay products because of cooking. Stong’s results showed that the activity size distribu- tion was trimodal (1.5 nm, 11 nm, 130 nm) before cooking and bimodal (11 nm, ll0 nm) during cook- ing. During cooking, the smallest mode (1.5 nm) disappeared, and this activity became associated with the 11 nm size range. In the same house, Strong (1989) made measurements in the living room while cooking in the adjacent kitchen. A trimodal size dis- tribution of radon decay products was observed, with the additional mode occurring at the 6 nm size range. This 6 nm mode may be due to the growth of aerosols from vapors generated during cooking. In Strong’s paper, no specific information was provided regarding the cooking process or the type of food cooked.

Ramamurthi and Hopke (1991) also conducted several measurements in another kitchen. They found an approximately 10 nm mode when the gas burners were operating. This small size range mode observed in the kitchen may be related to gas com- bustion of the gas burners.

The activity size distributions of radon decay pro-

ducts in the bedroom are presented in Figure 14. The activity in the 0.9 nm size range was found to be 50% for 218Po and 15% for 214Pb and 214Bi. The un- attached fraction of 218Po and PAEC decreased from 0.87 to 0.45 and reduced from 0.40 to 0.20. The equilibrium factor increased from 0.23 to 0.32, re- spectively. The fraction of all three distributions in the 1.5 to 5 nm size range was found to be 20%. For all three radon decay products there was very little activity in the 5 to 50 nm size range for all condi- tions. An increase from 20% to 50% in the 50 to 500 nm size range was observed for all three distribu- tions. As a whole, a bimodal size distribution was observed. For 218Po, the major mode was in the unat- tached cluster size range. For 214Pb and 214Bi, the minor mode was in the 2.8 nm size range and the major mode was in the 280 nm size range. The size distributions of the second and third measurements did not return to the background condition as did the distributions found after candle burning, cigar- ette smoldering, and vacuuming. It appears that the delay caused by the transport from the kitchen to the bedroom maintained the particle concentrations whereas when the particle sources were operated within the room, the particles were at their highest level at the end of the generating period. This pat- tern is also observed in the CN counts presented in Figure 15. The measurements and the results of the room and dose models are summarized in Table 6.

The PAEC and dose per Bq m-3 radon are shown in Figure 16. The reductions in the PAEC and the dose rate per Bq m-3 radon were quite different from the other experiments. The dose per unit radon showed a very slight average decrease of 4.6%. How- ever, given the uncertainty in both the measured and calculated quantities, the dose was essentially the same for the experiments with and without the air cleaner operating.

Conclusions Under normal conditions in the domestic environ- ment, the unattached fraction of PAEC can vary over a wide range (7%-40%). The equilibrium factor was between 0.13 and 0.50. However, these two quantities are strongly dependent on the situation measured in the house. Because of a large number of particles generated from normal household activities, the PAEC increased for a period of time and the unat- tached fiaction decreased. The particles generated from cigarette smoke and cooking dramatically shif- ted most of the radon progeny to the attached mode.

98 Li and Hopke: Air Filtration and Radon Decay Product Mitigation

1.0

0.8 e 0 4

2 0.6 rk x 3 0.4

.I

'ORu = 1149 Bq, m-' CN conc. = 20.600 cm-a

0 "'Po - 967 Bq m-' (1.6%)

230 Bq m-' (9.1%)

5l .r( 4 0 114 W = 0.6

rk A PAEC = 112 mWL (0.4%)

=Rn = 1038 Bq m-' CN Conc. = 7.000 cm-a - a 'laPo = 931 B q m-a (1.62)

L14

214 o Pb = 543 Bq m-' (1.3%)

- A Bi = 369 B q m-' (2.12) - A PAEC 138 mNL (0.3%) .

-

CN b n c . = 1 s . m em-'

123 '"Po - 606 Bq m-' (1.0%) 5l 3 Pb = 255 Bq rnJ (1.8%)

134 Bq m4 (4.22) 2 0.6 Bi = rs: A PMc 86 (0.52)

1 .o

0.8

5l 5 2 0.6 rk h 5 0.4 .-

x I I

~n = 1110 ~ g m - ~ m

CN Conc. = 7.000 cm-a

0 "'Po = -

887 Bq m-' (1.7%) 214

214 0 Pb = 510 Bq m-' (1.4%)

- A Bi = 410 m-' (1.Q%) A PMc = 136 mwL(O.3%) .

.

"." 1 10 100

Particle Diameter (nm)

During the cooking interval (first experiment).

1 .o Rn = 1331 Bq m

CN h n c . = IO.OOO cm- 0.8

e 0 "'Po = 1218 Bq m-' (1.3%) 0 Y Pb = 690 Bq m-3 (1.22) 0 0.6 A Bi = 312 Bq m-' (2.6%) rk A PAEC = 161 mWL (0.2%) x '6 0.4 3 <

.-

4

0.2

0.0 1 10 100

Particle Diameter (nm)

60 minutes after the cooking period.

1 .o

0.8 E 0

0 0.6

.d 4

& x 'g 0.4 4

0.2

0.0

-Rn = 1974 Bq m-' CN Conc. = 2,800 cm-' 0 ""Po = 1372 Bq m-3 (1.5%)

0 Pb = 554 Bq m-' (1.4%) A Bi = 507 Bq m-' (1.92) A PAEC = 165 mlL (0.3%)

C14

214

t I 1

1 10 100

Particle Diameter (nm)

135 minutes after the cooking period.

Particle Diameter (nm)

During the cooking interval (second experiment).

.i 4

3

0.0 -

1 10 100

Particle Diameter (nm)

60 minutes after the cooking period.

.. 4

Y 0.2

0.0 100 10 1

Particle Diameter (nm)

135 minutes after the cooking period. Fig. 14 Activity size distributions measured when particles were generated by cooking in the kitchen (bedroom door open) with the air filtration system.

Li and Hopke: Air Filtration and Radon Decay Product Mitigation 99

Table 6 Measurement, room, and dose model results for the cooking experiments with the air cleaner operating.

6 Z fi fP F PAEC X d q(U' Dose (~Gyhr' /Bqm-~) (Bq/m3) (103cm-3) (mWL) (hr-I) (nm) (hrl) Basal (1, h) Secretory(1, h)

( I ) 1149 20 0.333 0.198 0.361 112 10 26 4.2 10.1,26.4 22.0,57.5 (cleaner on for 7.5 hours, during cooking period)

1331 108 0.194 0.172 0.447 161 21 60 2.8 11.3,29.5 24.7,64.2 (60 minutes cooking)

1974 2.8 0.600 0.277 0.31 165 4.9 52 7.9 9.2,25.1 20.1,54.9 (135 minutes after cooking) (*I 752 15 0.633 0.234 0.321 65.2 4.1 20 4.1 10.0,26.5 21.8,57.8 (during the cooking interval)

1038 7 0.233 0.122 0.490 137 13 52 2.8 14.5,36.0 31.5,78.4 (60 minutes after cooking)

1110 7 0.484 0.189 0.453 135 7.4 37 5.1 13.8,35.8 30.1,78.0 (1 35 minutes after cooking)

These size distributions were stable for a long time after the aerosol generation. The particles pro- duced from candle burning and vacuuming were much smaller, with the average attachment dia- meters being around 15 nm. These particles did de- crease the unattached fraction. However, after 150 minutes, the size distributions had returned to the original background condition.

With the air filtration system operating without active aerosol sources, the unattached fraction of PAEC increased substantially to > 80%. The equi- librium factor was about 0.14. The PAEC reduction was about 60% with the bedroom door closed and only about 40% with it open. It appears that the in- creased circulation that occurred with the air cleaner operating and the door open substantially changed the infiltration rate of the attached activity into the room. The dose rate reduction for these two cases was essentially the same.

In the presence of active aerosol sources, the air

lo6 . . . . , I 1

I 0 Jan 26. 1990 v

1 0 Jan 27. 1990

5 [ , , . , _ , . . , _ _ _ _ 1 a 10' 0 25 50 75 100

Time (minutes)

Fig. 15 CN counts as a function of time during the cooking ex- periments with the air filter operating.

Cleaner On Cleaner Off

-.- 0 1 2 9

Time (hours)

4af J

0 1 e 3

Time (hours)

Fig. 16 Top: PAEC per unit radon concentration as o function of time from the start of the sample taken while cooking was being done in the kitchen with the door open.

Bottom: Dose per unit radon concentration 0 s a function of time from the start of the sample taken while cooking was being done in the kitchen with the door open.

100 Li and Hopke: Air Filtration and Radon Decay Product Mitigation

filtration unit typically reduced the concentration of particles within the hour following the end of par- ticle generation. After candle burning, cigarette smoking, and vacuuming in the bedroom, the re- ductions of PAEC by air filtration are about 60% with the air filtration system operating in the bed- room. During cooking in the kitchen, the reduc- tions of PAEC in the bedroom with the air filtration system were about 40%. However, for all cases the dose reductions were smaller than the particle and PAEC reductions. For those particles that were gen- erated within the bedroom, there was a 20% to 50% reduction in dose. In the case of cooking, where the door was open and particles infiltrated from the rest of the house, the dose reduction was only 5% on av- erage and appears to be insignificant. Thus, the dose reductions were lower than the reductions in activ- ity concentration, but there were no cases where the estimated dose actually increased.

Acknowledgements This work has been supported by the New Jersey Department of Environmental Protection through contact P32108 and by the U.S. Department of Ener- gy through Grant No. DE FG02 89ER61029. The collaboration and assistance of K. Gadsby, A. Caval- lo and R. Socolow of the Center for Energy and En- vironmental Studies at Princeton University is gratefully acknowledged.

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