accepted manuscript a comparison of methods to evaluate mass transport in damaged mortar

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Accepted Manuscript A comparison of methods to evaluate mass transport in damaged mortar Farnam Ghasemzadeh, Reza Rashetnia, Danny Smyl, Mohammad Pour-Ghaz PII: S0958-9465(16)30045-2 DOI: 10.1016/j.cemconcomp.2016.03.007 Reference: CECO 2616 To appear in: Cement and Concrete Composites Received Date: 3 April 2015 Revised Date: 13 February 2016 Accepted Date: 26 March 2016 Please cite this article as: F. Ghasemzadeh, R. Rashetnia, D. Smyl, M. Pour-Ghaz, A comparison of methods to evaluate mass transport in damaged mortar, Cement and Concrete Composites (2016), doi: 10.1016/j.cemconcomp.2016.03.007. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

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Accepted Manuscript

A comparison of methods to evaluate mass transport in damaged mortar

Farnam Ghasemzadeh, Reza Rashetnia, Danny Smyl, Mohammad Pour-Ghaz

PII: S0958-9465(16)30045-2

DOI: 10.1016/j.cemconcomp.2016.03.007

Reference: CECO 2616

To appear in: Cement and Concrete Composites

Received Date: 3 April 2015

Revised Date: 13 February 2016

Accepted Date: 26 March 2016

Please cite this article as: F. Ghasemzadeh, R. Rashetnia, D. Smyl, M. Pour-Ghaz, A comparison ofmethods to evaluate mass transport in damaged mortar, Cement and Concrete Composites (2016), doi:10.1016/j.cemconcomp.2016.03.007.

This is a PDF file of an unedited manuscript that has been accepted for publication. As a service toour customers we are providing this early version of the manuscript. The manuscript will undergocopyediting, typesetting, and review of the resulting proof before it is published in its final form. Pleasenote that during the production process errors may be discovered which could affect the content, and alllegal disclaimers that apply to the journal pertain.

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A Comparison of Methods to Evaluate Mass Transport in Damaged Mortar

Farnam Ghasemzadeha, Reza Rashetniaa, Danny Smyla, Mohammad Pour-Ghazb∗

a Graduate Research Assistant, Dept. of Civil, Construction and Environmental Engineering, North Carolina State University, Raleigh, NC, USA. b Assistant Professor, Dept. of Civil, Construction and Environmental Engineering, North Carolina State University, Raleigh, NC, USA.

Abstract:

The service life of reinforced concrete (RC) structures is directly influenced by the

transport properties of concrete. These transport properties are adversely affected by the

presence of cracks. Therefore, for accurate service life estimation of RC structures the effect

of cracks on mass transport needs to be understood and quantified. To quantify the effect of

cracks, different measurement methods have been developed. In this paper, we compare

different mass transport measurement methods for quantifying the effect of damage, and

investigate which method is more sensitive and provides the most information on the effect of

damage.

In this work, damage was induced by freeze-thaw in mortar specimens. Mass transport

properties were measured using electrical resistivity, rapid chloride permeability, sorptivity,

drying, air permeability, water permeability, and desorption isotherm. The results indicate

that the measured effect of damage depends on the mechanisms of transport used in the

measurement technique, and therefore, different measurement techniques do not necessarily

provide the same measure of the effect of damage. The water and air permeability are

comparatively more sensitive to the presence of damage.

Keywords: Cracking; Distributed Damage; Durability; Freeze-thaw; Transport Properties.

∗ Corresponding author Address: Dept. of Civil, Construction and Environmental Engineering, North Carolina State Univ., Campus Box 7908. 431C Mann Hall, Raleigh, NC 27695, USA. Email address: [email protected]

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1. Introduction

Distributed micro-cracking, referred to as damage hereafter, is commonly observed in

concrete structures. Damage may result from different deterioration processes, such as freeze-

thaw and alkali silica reaction. The presence of damage can significantly alter the transport

properties of concrete, adversely affecting the service life of structures. Therefore, in order to

account for the effect of damage on the service life of structures, its effects on mass transport

need to be quantified. Different methods have been developed to measure and quantify the

transport properties of cement-based materials. Many of these methods utilize different

transport mechanisms and, as such, provide different measures of the effect of damage on

mass transport properties [1]. We pose the following research questions: (i) how do different

measurement techniques show the effect of damage on mass transport? (ii) Which transport

measurement methods are more sensitive to the presence of damage? In line with these

questions, we experimentally compare different mass transport measurement techniques and

produce laboratory results that enable us to answer these questions.

Broadly, cracking in cement-based materials can be regarded as discrete cracking or

distributed cracking (damage). Researchers have investigated mass transport in cement-

based materials containing discrete cracks in fundamental works, such as the following:

Aldea et al. (1999) [2], who found that discrete cracks (40 -200µm crack widths) have a more

profound effect on water permeability than chloride permeability. Rodriguez (2001) [3]

showed that chloride diffusion increases in material with saw-cut simulated cracks and that

the lateral diffusion of chloride along the crack wall is nearly constant. Rodriguez and

Hooten (2003) [4] found that the depth of chloride penetration increases in cracked samples,

irrespective of the presence of mineral admixtures. Picandet et al. (2009) [5] found that crack

permeability increases with the cube of crack opening displacement in specimens with

discrete cracks in the range of 20-177 µm. They also concluded that the use of fibre

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reinforcement increases the tortuosity of cracks. Pour-Ghaz et al. (2009) [6,7] investigated

the role of saw-cut geometry as an idealized physical model of discrete cracks using X-Ray

radiography and numerical simulations; their results indicated that the geometry of cracks

significantly affects the ratio of the rate of unsaturated flow parallel and perpendicular to the

crack. Akhavan et al. (2012) [8] quantified the effects of tortuosity on the rate of flow in

saturated discrete cracks and found that water permeability increases with the square of crack

width and increasing tortuosity decreases water permeability by a factor of 4-6. Bentz et al.

(2013) [9] simulated the influence of transverse cracking on chloride penetration into

saturated concrete. They concluded that a simple 2-D simulation that considers diffusion may

provide a conservative estimate on the influence of cracking of the projected service life of

the concrete structures.

An early study investigating the effects of distributed damage on mass transport in

concrete was presented by Samaha and Hover (1992) [10]. In this study, distributed cracking

was induced by loading a specimen to 75% of its compressive strength; their results showed

that chloride mitigation, tested by the Rapid Chloride Permeability Test, increased by

approximately 20%. Breysse et al. (1994) [11] found that water permeability increases in

concrete with distributed cracking generated from tensile loading. Some examples of

continued research in this area include the works of Gérard and Marchand (2000) [12], who

developed a simulation model for distributed cracking in concrete, finding that the presence

of fracture networks increases diffusivity of cement-based material by a factor of 2-10. Yang

et al. (2006) [13] subjected concrete to freeze-thaw as well as compressive loading (up to

90% of the compressive strength), finding that distributed cracks resulting from both damage

mechanisms increased the connectivity of the fracture network, resulting in a reduction in

electrical resistivity and increased sorptivity of the materials. Torrijos et al. (2010) [14]

experimentally investigated the effects of ASR and thermally-induced cracking on concrete

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sorptivity. Their findings showed that sorptivity generally increases proportional to thermal

damage but deceases after a threshold value. Chunsheng et al. (2012) [15] used compressive

loading to induce distributed damage in concrete; these authors quantified damage using

ultrasonic pulse velocity and found that damage increases air permeability significantly,

while sorptivity and electrical resistivity were more strongly correlated to the total open

porosity than damage alone. Chunsheng et al. (2012) [16] continued previous work in [15]

finding that many transport properties, such as sorptivity, air permeability, electrical

resistivity, and effective porosity are significantly affected by crack density. M’Jahad et al.

(2014) [17] found that gas breakthrough pressure was a reliable indicator of damage presence

in concrete. Concrete with freeze-thaw damage was shown to increase the amount of

absorbed water and chloride penetration depth in Wang and Ueda (2014) [18]. Most recently,

Ghasemzadeh and Pour-Ghaz (2014) [1] investigated the effects of freeze-thaw damage in

concrete on transport mechanisms by providing experimental measurements and analytical

models describing the effects of damage. They concluded that measurement techniques that

are not based on the same transport mechanism will show the effects of damage on mass

transport differently. Ghasemzadeh and Pour-Ghaz (2014) [1] provided this argument mainly

based on their analytical models and suggested that further experimental work is necessary to

better understand how the observed effect of damage depends on the method of observation.

A brief summary of previous research on the effects of discrete and distributed fractures is

shown in Table 1. Note that, for brevity, only experimental works investigating the effect of

damage on specific mass transport mechanisms are included in Table 1.

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Table 1: Summary of previous studies on mass transport in cracked cement-based materials 1

Study Mechanism of cracking

Type of cracking

Type of materials

Measurement methods Highlights

Aldea et al. (1999) [2]

Split tensile load-induced cracking

Discrete Concrete Water and chloride permeability Water permeability is a more sensitive parameter, than chloride permeability, to crack width.

Rodriguez (2001) [3], Rodriguez and Hooten [4] (2001)

Split tensile load-induced cracking and saw-cut cracking

Discrete Concrete Water and chloride permeability Lateral chloride diffusion is roughly the same along the crack length, chloride diffusion increases in the presence of cracks, and water permeability is more significantly affected by crack presence than chloride diffusivity.

Picandet et al. (2009) [5]

Split tensile load-induced cracking

Discrete Concrete Gas and water permeability Cracks provide direct paths to convey a large portion of flow, with no influence from the degree of saturation. Permeability could be considered as an intrinsic parameter to evaluate the global effect of load-induced damage on concrete durability.

Pour-Ghaz et al. (2009a,b) [6.7]

Saw-cut crack Discrete Concrete Attenuation of X-Ray radiation the geometry of cracks significantly affects the ratio of the rate of unsaturated flow parallel and perpendicular to the crack

Akhavan et al. (2012) [8]

Split tensile load-induced cracking

Discrete Mortar Water permeability and image analysis on cracks

Permeability is a function of the square of crack width. Crack tortuosity and roughness reduce the permeability.

Samaha and Hover (1992)[10]

Compressive load-induced cracking

Distributed Concrete &

Mortar RCPT and Water absorption

The water absorption and chloride ion penetration differently reflect the effect of damage on transport properties of concrete as load levels increases.

Breysse et al. (1994) [11]

Tension-induced cracking (P.I.E.D.)

Distributed Concrete Water permeability Water permeability, measured perpendicular to tensile loading, is shown to increase as damage (load) increases.

Yang et al. (2006) [13]

Freeze-thaw loading Distributed Concrete Water absorption and electrical resistivity

Sorptivity increases linearly with damage; electrical conductivity increases in a bilinear fashion.

Torrijos et al. (2010) [14]

Low RH with high temperature and ASR

Distributed Concrete Water absorption and water permeability

Depending on the main transport mechanism, crack width, type of cracks and crack density differently affect the transport properties.

Chunsheng et al. (2012)[15]

Compressive load-induced cracking

Distributed Concrete Air permeability, sorptivity and electrical resistivity

While gas permeability correlated with damage, sorptivity and electrical resistivity correlated with open porosity – the connected pores available for fluid flow.

Chunsheng et al. (2012)[16]

Compressive load-induced cracking

Distributed Concrete Water absorption, gas permeability, electrical resistivity and crack geometry analysis

Crack geometry (i.e., length, orientation, and connectivity) and crack density have strong impact on transport properties.

M’Jahad et al. (2014) [17]

Freeze-thaw loading Distributed Concrete Mercury intrusion porosimetry, desorption isotherm, and gas breakthrough pressure

Gas breakthrough pressure seems to be a more sensitive indicator of damage than other studied methods.

Wang and Ueda (2014) [18]

Freeze-thaw loading Distributed Concrete Water absorption and chloride ion penetration

Water absorption and chloride penetration occurs at a higher rate in damaged specimens compared with undamaged concrete. The total amount of absorbed water in damaged specimens is more than undamaged specimens.

Ghasemzadeh and Pour-Ghaz (2014) [1]

Freeze-thaw loading Distributed Concrete Water absorption, electrical resistivity, desorption isotherm and saturated hydraulic conductivity

The rate of moisture transport increases with damage. The extent to which damage affects the rate of transport is dependent on the mechanism of transport. Saturated hydraulic conductivity is a much more sensitive parameter to damage due to the higher dependence of saturated hydraulic conductivity to crack width.

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Four conclusions can be drawn from the above literature review and the summary

provided in Table 1. (1) The effect of discrete cracking is better understood as compared to

the effect of damage. (2) It is unclear as to which transport mechanism, and subsequently

which measurement technique, is more sensitive to the presence of damage. (3) The majority

of these studies have used only a few mass transport measurement methods and, to the

knowledge of the authors, the effect of damage has not been interpreted in the light of

transport mechanisms used in these measurement methods. For example, it has been shown

that while cracking can increase water permeability several orders of magnitude [19],

diffusivity is less affected by cracking [2,3,4,18], but the relationship of the data to the

mechanisms of mass transport was not discussed. (4) The sensitivity of different methods to

the presence of damage is not discussed in the previous works.

The present work aims to develop a better understanding of the effects of damage on mass

transport in damaged cement-based materials by investigating the mechanisms of mass

transport involved. In this work, damage was induced by freeze-thaw loading in mortar

specimens. Active acoustic emission (AE) was used to quantify the degree of damage.

Passive AE was also used to monitor damage formation during the freeze-thaw cycles.

Electrical Impedance Spectroscopy (EIS) and four-electrode Wenner methods were used to

measure the bulk and surface electrical resistivity, respectively. Rapid Chloride Permeability

Test (RCPT), sorptivity, drying, air permeability, water permeability, and desorption

isotherm measurements were also carried out. In the following sections, the materials and

methods used are described. Then, the results are presented and discussed. Finally, the

conclusions of this study are presented.

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2. Materials and Specimen Preparation

2.1. Mixture proportioning and specimen preparation

The mortar mixture was made with Ordinary Type I Portland Cement (OPC) and had a

water-to-cement ratio (w/c) of 0.42. The fine aggregate consisted of natural river sand with a

fineness modulus of 2.65 and a maximum aggregate size of 2 mm. The fine aggregate mainly

consisted of silica and had 0.90% saturated surface dry (SSD) moisture content. The cement,

aggregate, and water reducer content in the mixture were 609 kg/m3, 1466 kg/m3, and 0.50

kg/m3, respectively. The mortar mixture was prepared following ASTM C192 [30].

The mortar mixture was cast in 102 mm x 204 mm cylindrical molds. Mortar cylinders

were kept sealed for the first 24 hours and were then demolded and cut into appropriate

geometries (for different experiments as discussed below in Table 2) using a diamond-tipped

wet saw. Top and bottom ends of the cylindrical specimens (roughly 25 mm) were cut and

discarded to minimize the possible end-effects. While cutting the specimens may result in

microcracking close to the cut surfaces, this damage is significantly smaller than the damage

due to freeze-thaw which was monitored as described later. All of the specimens were cured

in lime-saturated water at 25±1ºC for 18 months after cutting to achieve high degree of

hydration, a uniform saturation, and a uniform initial condition.

2.2. Number of Specimens Used in Each Test

A large number of tests were performed in this work. A detailed description of each test is

provided in the Methods Section. Table 2 reports the total number of specimens and the

number of replicates used in each test. All tests included a set of reference specimens (with

no damage) with the same number of replicates indicated in Table 2. The dimensions of the

specimens used in each test are also reported. The size of the specimens for each test method

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was chosen based on the standard test method or previously published literature when

applicable. It should be noted that the dedicated specimens were made for each test and

specimens were not used in multiple tests. Furthermore, dedicated specimens were made for

each degree of damage in each test, except for acoustic emission and surface resistivity where

measurements were performed on the same set of specimens at all degrees of damage due to

the non-invasive nature of these tests. All the specimens had the same age at the time of

testing.

Table 2: The number of specimens, number of replicates, and specimen dimensions used in each test

Test Method Specimen Information

Total Number of specimens

Number of Replicates*

Diameter [mm]

Thickness [mm]

Acoustic Emission (AE) 6** 3** 102 25 and 50 Rapid Chloride Permeability Test (RCPT)

24§ 4 102 50

Electrochemical Impedance Spectroscopy (EIS)

24§ 4 102 50

Surface Resistivity (SR) 3** * 3** * 102 204 Sorptivity 12§§ 2 102 25 Drying 12§§ 2 102 50 Air permeability 18§§§ 3 102 25 Water Permeability 24§ 4 102 25

Desorption isotherm 8£ 2 Specimens with 0.50-1.5 mm thickness and 50-100 mg weight€

*Indicates the number of samples for each degree of damage. ** Due to the non-invasive nature of the test the same set of specimens were monitored during the freeze-thaw loading. Two different sample thicknesses were used with three replicates for each thickness. *** Due to the non-invasive nature of the test the same set of specimens were monitored during the freeze-thaw loading. §Five degrees of damage and a set of reference with four replicates (6x4 = 24). §§Five degrees of damage and a set of reference with two replicates (6x2 = 12). §§§Five degrees of damage and a set of reference with three replicates (6x3 = 18). §§§Three degrees of damage and a set of reference with two replicates (4x2= 8). €Specimens were cut from the center of 25 mm x 102 mm disk using a precision Scanning Electron Microscope wet-saw.

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3. Methods

3.1. Freeze-thaw loading

Freeze-thaw loading was performed in an air-cooled chamber. Each cycle was 4 hours in

duration including a cooling period from 21˚C to -35˚C, and a heating period back to 21˚C.

The cooling and heating periods included two ramps as well as two constant temperature

periods (temperature profile shown Figure 1). These constant temperature periods were

designed to allow the specimen to equilibrate with the surrounding air, decreasing the

temperature gradient across the samples. This freeze-thaw loading profile was chosen

following references [1, 31]. The core temperature of a set of specimens was monitored using

embedded thermocouples. Type K thermocouples with an accuracy of 0.1oC were used. To

keep the specimens saturated, during the freeze-thaw testing, they were wrapped in a water

saturated cloth and then were sealed with a thin layer of plastic sheet [31]. A total of 25

freeze-thaw cycles were used and a set of specimens were removed from the chamber for

testing after 2, 5, 10, 15, and 25 cycles.

3.2. Acoustic Emission

Cracking and permanent deformation of materials results in the release of strain energy.

The released strain energy, in turn, leads to the generation and propagation of elastic stress

waves. These stress waves cover a wide range of audible and inaudible frequencies and are

known as acoustic waves. Passive AE describes a technique that captures and digitizes the

acoustic waves in the form of electric signals at the surface of a material or structure. To

convert the captured acoustic waves into electrical signals, piezoelectric sensors are used. In

this work, passive AE was used to continuously monitor damage formation and cracking

during the freeze-thaw cycles. Circular AE sensors with a peak frequency of 375 kHz were

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used. The diameter of the piezoelectric surface of the AE sensors was 2.00 cm. A Vallen

AMSY-6 acoustic emission equipment set with VS375 sensors manufactured by Vallen

Systeme were used.

In this work, active AE was used to monitor the damage in mortar specimens at the end of

a predefined number of freeze-thaw cycles (Fig. 2). Active AE describes a method in which a

series of pulse (a total of four discrete pulses in this work) is sent by an AE sensor and is

captured by another sensor (pitch-catch). Then, the order of sending and receiving the pulses

is switched between the two sensors. The transmission time is measured for each pulse and

the average value is reported (average of eight transmission times). While similar to

Ultrasonic Pulse Velocity measurements, the active AE measurements are generally more

sensitive due to the high frequency of the AE sensors. In this work, active AE measurements

were performed using the same sensors and equipment set used in passive AE measurements.

To mount the AE sensors on disk specimens, flat surfaces were created on the perimeter of

the circular disk specimens by trimming the specimen perimeter (tangent to the perimeter).

Due to the small size of the sensors, only a maximum trimming depth of 5 mm was necessary

which only negligibly affected the circular shape of the disk. AE sensors were coupled to the

specimen using vacuum grease at 180o with respect to each other, performing measurements

along the diameter of the specimen. Specimens were placed on a layer of acoustic mat resting

on a rigid stainless steel frame which was isolated from the chamber to minimize vibration

and noise. A stainless steel rod was also used as a reference specimen to monitor the

environmental noise during the test and to ensure that the coupling agent did not degrade

during the freeze-thaw cycles [31]. Further detailed information regarding the application of

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AE system on damage monitoring in cement-based materials can be found elsewhere [1, and

31-34].

3.3. Rapid Chloride Permeability Test (RCPT)

Rapid chloride permeability test (RCPT) is often used as an indirect measure of material

permeability. In this test, a constant potential difference (typically 60 volts) is applied across

a concrete disk specimen, through solutions of sodium hydroxide and sodium chloride on two

different sides of the specimen, and the amount of electric charge passing through the

specimen is measured by monitoring the current required to maintain the constant potential

difference. The total amount of electric charge passed through the specimen is then estimated

based on the measured current during the first six hours of the test. The total charge (in

coulombs) is then used as an indirect measure of permeability. In the present work, RCPT

was performed according to ASTM C1202 [35] using an in-house developed equipment set

meeting all of the specifications of ASTM C1202.

3.4. Surface Resistivity

In this work, surface resistivity was measured using a four-electrode Wenner probe on 102

mm x 204 mm cylinders. The equipment utilized a 40 Hz alternating current (AC). Note that

the ends of the specimens used for surface resistivity were not cut. This however does not

affect the measurements since the distance between the outer two electrodes of Wenner probe

equipment was smaller than the total length of the cylinder, and therefore, the Wenner probe

measured the average properties between the outer two electrodes (i.e., the results are not

influenced by the end of the specimens) [36]. Before measurements, specimens were taken

out of the chamber and were kept in a large water container until they reached thermal

equilibrium with the ambient temperature (approximately 24 hrs). Note that, the specimens

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were not taken out of the plastic wrap before placing them in the water tank. Therefore, the

plastic wrap prevented entry of extra water into the specimen. After each measurement,

specimens were placed back in chamber to undergo the same number of freeze-thaw cycles as

other specimens.

3.5. Electrical Resistivity

The bulk electrical resistivity measurements were performed on 50 mm thick disk

specimens. Three different arrangements were used in measuring bulk electrical resistivity.

First, the specimens were sandwiched between two stainless steel plate electrodes and, to

improve electrode contact, a copper sulphate based conductive gel was used. Stainless steel

plate electrodes were connected to the EIS equipment [36, 37]. Second, specimens were

installed in a RCPT cell and EIS was used to measure the bulk resistivity [38]. Finally, the

initial currents from the RCPT measurements were utilized to measure the bulk electrical

resistivity [39]. Note that in all three measurement arrangements, the direction of the

measurement was perpendicular to the circular cross-section of the specimen. To provide a

better comparison, the same specimens were used in all three measurement arrangements for

each degree of damage. EIS measurements were performed with amplitudes of 500 mV over

the frequency range of 1.0 Hz to 1.0 MHz. Before measurements, specimens were kept in a

large water container while wrapped in plastic sheets until they reached to thermal

equilibrium with the ambient temperature (6-8 hours).

3.6. Sorptivity

The sorptivity test, in general, describes the upward water absorption by capillary suction

in concrete. To measure the amount of the absorbed water by the specimen, the specimen is

placed in contact with water and the mass of the specimen is monitored over time. In this

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work, water absorption was carried out following ASTM C1585 [40] on 25 mm thick disks.

The perimeter of the specimens were sealed using epoxy coating. To avoid contamination of

circular cross-sectional surfaces with epoxy, they were covered with pieces of paper during

the application of epoxy. The top circular cross-sectional surface that was not in contact with

water was covered with a loose layer of plastic that was secured to the specimen with a

rubber band as specified by ASTM C1585 and similar to the works by Castro [41, 42]. The

measurements were carried out up to 150 days.

3.7. Drying test

The drying rate of mortar specimens with different degrees of damage were measured by

monitoring mass loss in a chamber with a relative humidity of 50 ±5 % at 23±1°C. Prior to

weight loss measurements, specimens were saturated under high vacuum (0.015 mm

Mercury). Weight loss was continuously recorded with one minute intervals for the first 10

hrs using an automated digital scale and then the measurements were continued daily, up to 7

days, and weekly up to 60 days. Only one surface of the sample was subjected to drying and

all other surfaces were sealed using epoxy coating.

3.8. Air Permeability

The air permeability of mortar specimens were measured using the method outlined in [43,

44]. In this method, a circular disk specimen is placed against a cylindrical chamber of

known volume. The air in the chamber is evacuated to a known pressure using a vacuum

pump. Then, the pressure drop in the chamber is monitored as a function of time while air

permeates through the specimen. In this work, a vacuum pressure of 736 mm Hg was induced

and the time to reach to 635 mm Hg was measured. Depending on the permeability of the

specimens, measurements were completed in 1 to 30 minutes. To ensure air tightness of the

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equipment seals, initial tests were performed on a 25 mm thick aluminium disk and no

pressure decay was observed for 24 hours.

The circumference surface of the specimens was coated with a rapid-setting epoxy to

induce one-dimensional air flow through the circular cross-section of the disk. All the

specimens were dried in an oven at 50+2°C for 48 hrs before the measurements. This

essentially resulted in complete drying of the specimen eliminating the effect of initial

moisture content of the samples while minimizing additional cracking since this drying does

not produce large temperature gradients across the specimen [45]. A thin strip of soft clay

was also used to seal the chamber to the face of specimen.

The Boyle-Marriotte law was used to calculate the air permeability assuming that the

specimen is a homogeneous porous material. Air permeability index is calculated per Eq. 1

[44].

������ =� − ����

�∆�� �� −������ �

�� ��. 1

where ������ is the air permeability index (m2/s), � and are the initial and final vacuum

pressure in the chamber (Pa) respectively, �� is the volume of vacuum chamber (m3), ∆� is the

duration of measurement (s), � is the atmospheric pressure (Pa), � is the thickness of

specimen (m), and � is the cross sectional area of the specimen (m2).

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3.9. Water Permeability

Water permeability describes flow of water through water-saturated porous material under

a pressure gradient. In this work, measurements were performed using in-house developed

equipment. The details of the water permeability equipment are discussed in the previous

study by the authors [1]. Briefly, this equipment works by measuring the pressure of a

column of water on top of the specimen using an ultra-sensitive pressure sensor. As the water

permeates in the porous material, the pressure drops and permeability of material can be

calculated using this pressure drop. All measurements were performed at 23±1°C.

3.10. Desorption Isotherm

The desorption isotherm of mortar specimens with different degrees of damage were

measured using an automated vapour sorption analyser (Q5000SA manufactured by TA

Instruments). The measurements were performed at 23˚C. In each measurement, the

specimen was equilibrated at 97.5% RH (relative humidity) and the RH was sequentially

dropped from 97.5% to 0% RH, in 5% RH increments to 2.5% and then to zero RH. The

sample was held at each RH step until it reached to equilibrium. The equilibrium was defined

as a mass change less than 0.001mg within 15 min [46]. This equilibrium criterion is tested

and validated based on the extensive works in [31, 37, 42, 46, and 47]. The specimens were

0.50-1.5mm thick and 50-100mg in weight. A full description of desorption isotherm

experiment using automated sorption analyser has been discussed in [31, 37, 42, 46, and 47].

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4. Results and Discussion

4.1. Acoustic Emission

Figure 1 illustrates the results of passive AE testing during the freeze-thaw cycles. Figure

1a and 1b show the AE peak amplitude distribution during the first and the last 5 freeze-thaw

cycles for mortar disks with 25 mm thickness. Figure 1c shows the total number of AE hits in

each freeze-thaw cycles for 25-mm thick samples. The same plots presenting the results for

50-mm thick samples are shown in Figs. 1d, 1e, and 1f respectively. Clearly, in Figs. 1c and

1f a higher numbers of hits are captured during the first few cycles as compared to the

subsequent cycles, signifying that a large number of cracks develops in the first few freeze-

thaw cycles and the rate of formation of cracks decreases in subsequent cycles [1, 31].

Figure 2 shows the degree of damage measured with active AE after a given number of

freeze-thaw cycles. The degree of damage (D) is calculated based on the wave travel time in

damaged and undamaged specimens using � = 1 −�� �⁄ �� where � and � are wave

transmission time in undamaged and damage material respectively. In Fig. 2 results for

specimens with 50 mm and 25 mm thickness are labelled by AE-50 and AE-25 respectively.

Note that the error bars in Fig. 2 show the range of the measurements. A linear increase of

damage with the number of freeze-thaw cycles is observed. Slightly higher damage is

observed in 25-mm thick samples. This may in part be a result of a lower core temperature in

25-mm thick disks as compared to 50-mm thick samples.

Note that while in Fig. 2 damage increases approximately linearly with the number of

cycles, the number of AE hits significantly decreases in later cycles as seen in Figs. 1c and 1f,

the latter indicating the reduction in the rate of development of new cracks. This observation

is consistent with previous study by the authors which indicates that in the later freeze-thaw

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cycles (or higher degrees of damage) the average crack width increases with a higher rate as

opposed to the formation of new cracks. In fact, the increase of degree of damage at higher

damage levels can be mainly attributed to the increase in the crack width. An analytical

model to describe this was previously presented in [1]. In addition to increased crack width,

crack density increases, resulting in crack network percolation. Crack network percolation

results in a high degree of damage.

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Figure 1: Damage formation during the freeze-thaw loading monitored by passive acoustic emission: (a) peak amplitude distribution during the first 5 cycles in 25-mm thick samples, (b) peak amplitude distribution during the last 5 cycles in 25-mm thick samples, (c) the total number of AE hits in each freeze-thaw cycle in 25-mm thick samples, (d) peak amplitude distribution during the first 5 cycles in 50-mm thick samples, (e) peak amplitude distribution during the last 5 cycles in 50-mm thick samples, (f) the total number of AE hits in each freeze-thaw cycle in 50-mm thick samples.

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Figure 2: Damage measured using active acoustic emission.

4.2. Rapid Chloride Permeability Test (RCPT)

Figure 3 illustrates the results of RCPT for specimens with different degrees of damage.

Figures 3a and 3b show the current flow over time and the total charge passed (coulombs),

respectively. In both Figs. 3a and 3b the error bars indicate the full range of measurements

(maximum and minimum). In Fig. 3a while the current continuously increases over time at

low damage levels, at higher damage levels current initially increases and then decreases.

This reduction of current at later times affects the total charge passed in specimens with

higher damage levels: in Fig. 3b the total charge passed increases with damage and then it

reaches to a plateau at high degrees of damage. Consequently, the difference between the

total charged passed from D=25.21% to D=44.09% is rather insignificant, making the

reliability of RCPT questionable at high damage levels.

There are three possible explanations for the observed plateau in Fig. 3b. First, in high

damage levels, the chloride concentration reduces in the NaCl solution cell due to the rapid

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transfer of high amount chloride ions to NaOH solution cell. This in turn reduces the amount

of current transfer by chloride ions through the specimen. Second, the chloride concentration

may be reduced in the system due to the chloride binding of hydration products [48]. In the

presence of high degree of damage, a higher amount of chloride ions can move into the

specimen, thus increasing the chance of chloride binding, and therefore, decreasing the

amount of current transfer by chloride ions [49]. Third, during the chloride binding a portion

of chloride ions can be replaced by the OH ¯ ions. Once OH ¯ ions are released, simultaneous

diffusion and migration occurs, and therefore, OH ¯ ions could either move to the catholyte

solution (NaCl solution) side through diffusion mechanism or to the anolyte solution (NaOH

solution) side through the migration mechanism [50]. The OH ̄ ions movement mechanism

depends on the concentration of OH ¯ ions in the pore solution. According to the results in

Fig. 3, it seems that the OH ¯ ions movement mechanism changes into diffusion mechanism

in specimens with high damage levels, thus reducing the current passed through the

specimen. It should be also noted that specimens were kept 18 months in lime-saturated

water and it could be safely assumed that cement particles were well hydrated. Therefore,

healing of the cracks could not be a potential contributor to the current reduction in damaged

specimens.

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Figure 3: The results of Rapid chloride penetration test (RCPT): (a) current flow during the

test, (b) total change passed.

4.3. Electrical Resistivity

Figure 4a illustrates the normalized bulk resistivity of mortar specimens measured using

the three bulk resistivity measurements discussed in Section 3.5 (i.e., stainless steel plates

with EIS, RCPT cell with EIS, and using initial RCPT current). The results are normalized to

the initial resistivity of the undamaged specimen. In all three sets of measurement, the

normalized bulk resistivity decreases with damage. The error bars in Fig. 4a and 4b show the

range of measurements. Resistivity decreases with a high rate initially when a large number

of cracks form in the specimens. With further increase of damage, the electrical resistivity

decreases with a lower rate, consistent with AE results. The results obtained using stainless

steel plates show a lower resistivity at all damage levels as compared to other methods. This

is mainly due to reduced contact impedance when conductive gel is used in measurements

[51].

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Figure 4: (a) Normalized bulk electrical resistivity, to the resistivity of undamaged mortar

measured using stainless steel plates with EIS, using RCPT cell with EIS, and using initial

RCPT current, (b) normalized surface resistivity as a function of damage.

Figure 4b illustrates the normalized change of surface resistivity with damage. It should be

noted that the degrees of damage were not measured for these cylinders and we have assumed

the same degree of damage for the cylinder specimens and 50-mm thick disks at equal

number of freeze-thaw cycles. While this may not be a completely correct assumption, it

provides a first order approximation. In Figure 4b the normalized surface resistivity decreases

with increase of damage with a similar trend observed in bulk resistivity in Fig. 4a. While

there is a slight difference between the bulk and surface measurements, the simplicity of

surface resistivity measurements potentially put forward the idea that this technique might be

used to evaluate freeze-thaw damage on cement-based materials provided the boundary

conditions and temperature effects are well controlled. More investigation, however, required

to correlate surface resistivity to damage.

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4.4. Sorptivity

Figure 5 illustrates the results of water absorption during the first 150 days. Figures 5a

shows the volume of the absorbed water (mm3) normalized to the surface area of the

specimen (mm2) as a function of square root of time. Figure 5b shows the same results

presented in terms of degree of saturation. Figure 5a shows that the total water absorption

increases with damage, indicating the physical change in pore structure [1]. Also, at early

stages of water absorption, the rate of water absorption increases with damage. Furthermore,

in Fig. 5a, specimens with high levels of damage plateau more rapidly. This observation

indicates that unsaturated cracks and capillary pores are rapidly filled with water, and then,

water diffuses into the larger air voids. Figure 5b also shows that specimens with high level

of damage reach to higher degree of saturation earlier as compared to specimens with a lower

level of damage.

Figure 5c illustrates the normalized initial and secondary sorptivity of the damage

specimens (normalized to the initial and secondary sorptivity of the undamaged samples,

respectively). Both normalized initial and secondary sorptivity are indicated by S/So on the

vertical axis. The initial sorptivity is the slope of the first linear region of the sorption test in

Figure 5a, and the secondary sorptivity is the slope of the second (late stage) linear region in

Figure 5a. Figure 5c shows that initial sorptivity increases almost linearly with increase of

damage. The secondary sorptivity, however, initially decreases with an increase of damage at

low damage levels, and then, remains constant at higher damage levels. It seems that the

secondary sorptivity is independent of degree of damage at high levels of damage. Authors

have previously discussed that cracks change water absorption mechanism in damaged

specimens [1]. Briefly, in the initial phase of water absorption, cracks act as capillary tubes

that absorb water rapidly, provide access to capillary pores away from the exposed surface,

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and provide access to large air-filled voids. At later stage, air diffusion and dissolution

mechanisms play a more significant role in water absorption [1, 52].

Figure 5: (a) Water sorption of mortar specimens with different degrees of damage during the

first 150 days; (b) water sorption results expressed in terms of degree of saturation for mortar

specimens with different degrees of damage; (c) normalized initial and secondary water

sorptivity of mortar specimens as a function of damage.

4.5. Water and Air Permeability

Figures 6a and 6b illustrate the results of air permeability and water permeability

measurements, respectively. Both results are normalized to the respective permeability of the

undamaged mortar. Note that in Fig. 6a, K(air) is air permeability index as opposed to the

actual permeability. The results in Figs. 6a and 6b show that air and water permeability

exponentially increase with damage. The rapid increase of air and water permeability with

damage can be attributed to the high volume of crack density, increase in crack width, and

crack percolation.

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Figure 6: Normalized permeability of damaged specimens to the permeability of

undamaged specimen: (a) air permeability, and (b) water permeability.

4.6. Drying

Figure 7 illustrates the results of the drying test presented in terms of total remaining water

in the specimens as a function of square root of time (to better illustrate the water loss at early

ages). In Fig. 7, it is observed that the rate of drying increases with damage since cracks

provide paths for water to migrate to the surface. This mechanism is commonly referred to as

the wicking [53]. Once water dries from the surface, cracks start to drain the interior water in

cracks and capillary pores. From Fig. 7, it seems that once all the water in cracks is wicked to

the surface, the mechanism of drying changes to the diffusion of water vapour. However,

there is certainly some overlap between these two mechanisms in a transition period.

It is also important to note that in Fig. 7, the total amount of water present in the samples

increases significantly with damage. In Table 3, the saturation water content, the residual

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water content (the remaining water at the end of drying experiment after 60 days), and the

amount of evaporated water (difference between initial and residual water) are provided for

specimens with different degrees of damage. The saturation and residual water were

determined by drying specimens in an oven at 50˚C for two days (different samples were

used). As shown in Table 3, specimens retain significantly more water in the cracks as

damage increases, resulting in supplying more water to the surface of specimen during drying

test, and consequently, increasing the rate of drying.

Figure 7: Weight loss due to evaporation of water from mortar specimens with different

degrees of damage during the first 60 days.

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Table 3: Change in water content in specimens with different degrees of damage.

Damage

Amount of water in different conditions (g)

Water content at Saturation

Residual Water Evaporated

Water 0.00% 30.92 17.74 13.18

3.17% 35.26 18.86 16.4

7.57% 49.00 18.1 30.90

14.00% 59.37 21.25 38.12

25.21% 63.95 22.72 41.23

44.09% 69.72 25.42 44.30

4.7. Desorption Isotherm

The desorption isotherm of specimens with different degrees of damage are shown in the

Figure 8. Clearly, the water content gradually increases with damage at intermediate relative

humidity values, followed by a rather large increase at high relative humidity values. The

higher water content in mortar specimens with higher levels of damage can be explained by

the contribution of cracks acting as capillary porosity and retaining more water within the

material. The desorption isotherms can be used to provide a quantitative measure of size

distribution of the cracks. Note that, however, the desorption isotherms are obtained up to

97.5% RH, while cracks within the samples cover equivalent crack widths (Kelvin radius)

much larger than that corresponding to relative humidity of 97.5%. Therefore, the entire

information about the crack distribution is not necessarily included in the isotherms in Fig. 8.

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Figure 8: Desorption isotherm of mortar specimens with different degrees of damage.

5. Evaluating Transport Measurement Methods

Results of the laboratory tests on moisture transport in mortar specimens with different

degrees of damage shows that transport measurement methods reflect the effects of damage

differently. Table 4 summarizes how each measurement technique shows the effect of

damage. Depending on the mechanism of mass transport used in the measurement, the effect

of damage changes significantly. It can be seen that RCPT and electrical resistivity are not

sensitive methods at high damage levels (above 20% damage) while total amount of charge

measured with RDPT and electrical resistivity linearly vary with damage at low damage

levels (below 20% damage). Initial sorptivity increases linearly with damage in the entire

range of damage measured in this work, but secondary sorptivity initially decreases with

damage (up to 10% damage) and then remains approximately constant at all damage levels.

Finally, both air and water permeability increase exponentially with damage.

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Table 4: Comparison of different transport measurement methods

Method Effect of Damage Mechanism of measurement

Rapid Chloride Penetration Test (RCPT)

Linearly increases at low damage levels; remains approximately constant at high damage levels

Electrophoresis

Electrical resistivity (EIS and surface resistivity)

Decreases at a high rate at low damage levels and decreases with a low rate at high damage levels

Electrical conduction (AC current)

Sorptivity Initial sorptivity increases linearly with damage; secondary sorptivity initially decreases with damage and then remain constant at higher damage levels

Capillary suction

Drying The initial rate of drying increases with damage increase

Moisture diffusion

Air permeability Air permeability exponentially increases with damage

Flow under pressure gradient

Water Permeability Water permeability exponentially increases with damage

Flow under pressure gradient

Desorption isotherm

The water content gradually increases with damage at intermediate RH values, followed by a larger increase at high RH values; generally does not account for all crack widths

----

6. Conclusion

In this paper, we posed the following questions: (i) How do different measurement

techniques show the effect of damage on mass transport? (ii) Which transport measurement

method is more sensitive to the presence of damage? To this end, we experimentally

measured the effect of damage, induced by freeze-thaw loading in mortar samples, using

different mass transport measurement techniques. It was observed that mass transport

increases with damage irrespective of the measurement method. However, different

measurement methods differently reflect the effect of damage on mass transport depending

on the mechanism of transport utilized in the measurement method. Different methods also

show different sensitivity to the presence of damage. Rapid chloride permeability test and

electrical resistivity are only sensitive at low damage levels (below 20%). Initial sorptivity

increases linearly with damage at all levels. Water and air permeability increase

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exponentially with damage and seem to be the most sensitive parameter to the presence of

damage.

Acknowledgments

This work was conducted in the Materials and Sensor Development Laboratory (MSDL)

and Constructed Facilities Laboratory (CFL) at North Carolina State University. The authors

would like to acknowledge the support which has made these laboratories and this research

possible.

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