Original citation: Ling, T.-C., Poon, C.-S., Lam, W.-S., Chan, T.-P., Fung, K.-L.

(2013) X-ray radiationshielding properties of cement mortar prepared with different types of aggregate. Materials and Structures, In Press, Available online October 2012 http://www.springerlink.com/content/81x4385458x030m8/

X-ray radiation shielding properties of cement mortars prepared with different types of aggregates
Tung-Chai Ling,1,2 Chi-Sun Poon,1* Wai-Shung Lam,1 Tai-Po Chan,1 Karl Ka-Lok Fung1
1

The Hong Kong Polytechnic University, 2University of Birmingham

Abstract The types of aggregate used play an important role in determining the effectiveness of xray radiation protection of cement mortars. Cement mortars were prepared using fine aggregates obtained from six different sources. The influence of aggregate type on x-ray shielding properties was studied. The results showed that mortars prepared with barite and lead-laden recycled cathode ray tube (CRT) funnel glass provided better shielding properties than mortars prepared with natural sand, natural crushed fine stone or crushed beverage glass. This is attributed to the use of dense aggregates being able to interact with x-ray radiation, thus reducing the depth of penetration. Due to the superior shielding properties of the mortar containing barite, it can be used to replace traditional sand mortar for applications as rendering or plastering materials for the construction of medical diagnostic and CT scanner rooms. Keywords: cement mortar, radiation shielding, waste recycling, recycled aggregate, funnel glass. 1. Introduction X-ray radiation shielding is based on the principle of attenuation, which is the ability to block or reduce the intensity of radiation through photoemission and scattering by a barrier material. Portland cement concrete has been known for decades as a polyphase composite material for the purpose of radiation shielding [1-5]. Unlike other barrier materials, concrete is a strong, durable and relatively inexpensive material to produce and easy to form, making it more popular and widely used in construction works. Also, the aggregate particles contained in a matrix of Portland cement paste have many of the physical qualities that make it suitable for radiation shielding [4]. It is generally agreed that the use of heavyweight aggregate can significantly improve the radiation shielding properties of concrete. Several research studies have been done to investigate the effect of different types and amounts of aggregate used in concrete for gamma radiation shielding [6-9]. Sakr [8] compared the shielding behaviour against gamma-rays between concrete prepared with ilmenite, barite and gravel. It was found that *First author: t.ling.1@bham.ac.uk; tcling611@yahoo.com Page 1

the aggregate type is the main factor affecting the density and thus the radiation attenuation coefficient. He concluded that ilmenite concrete provided the best shielding properties, followed by barite concrete and gravel concrete. Akkurt et al. [1] found that the type of aggregate used in concrete was more important than the replacement rate in affecting gamma-ray shielding. Akkurt et al. [9] prepared concrete with different percentages of zeolite aggregate and found that the linear attenuation coefficient decreased with increasing zeolite rate, which was probably due to the porous structure of the zeolite that led to low-density concrete. Therefore, zeolite was not recommended to be used in concrete for the purpose of gamma radiation shielding. There are only a few studies on developing and optimizing construction materials as a shield against x-ray radiation. It is therefore of interest develop cement mortar that can provide high levels of radiation shielding ability by the incorporation of different types of aggregate. In this study, six different types of aggregate were assessed. The basic properties of the cement mortars, such as flexural strength, compressive strength and hardened density were first evaluated before the radiation shielding properties were assessed. 2. Experimental details 2.1. Raw materials Six different types of fine aggregate (Fig. 1) with a particle size less than 2.36 mm were used as follows: 1) Sand, a river sand sourced from the Pearl River. 2) Fine stone (FS), a crushed aggregate (granite) sourced from a local quarry. FS has been widely used as a fine aggregate in the construction works in Hong Kong. 3) Beverage glass (BG), crushed beverage glass cullets derived from post-consumer glass bottles (soda-lime) and obtained from a local glass recycling plant. In Hong Kong, the BG is mainly used in non-structural concrete products. 4) Funnel glass-untreated (FG-U), derived from dismantled cathode ray tubes (CRT) glass and crushed into particle sizes similar to sand. The crushed FG-U contained an average lead (PbO) content of 22-25% wt. FG-U was obtained from a local CRT glass waste recycling centre. 4) Funnel glass-treated (FG-T), an acid treated FG-U. The treatment process was carried out by immersing FG-U in 5% nitric acid solution for 3 h to extract the lead on the glass surface. The treated glass was washed with water before use. 6) Barite, a crushed heavyweight aggregate with a density of about 4.10 kg/m3 sourced from a quarry in Hunan, China. The physical properties of the studied fine aggregates are presented in Table 1. ASTM Type I ordinary Portland cement (OPC) and fly ash complying with ASTM class F ash were used as cementitious materials. The fly ash content was kept constant at 25% of the total cementitious materials following our previous study [10]. Our previous results demonstrated that under such conditions, the expansions due to the alkali-silica reaction (ASR) were reduced to an innocuous behavior according to ASTM C 1260 (below *First author: t.ling.1@bham.ac.uk; tcling611@yahoo.com Page 2

0.10%) even 100% beverage glass [11-12] or 100% CRT glass [10, 13] were incorporated in the mix.

Sand

Fine stone

Beverage glass (cullets)

Funnel glass (treated)

Funnel glass (untreated)

Barite (heavyweight)

Fig. 1. Photographs of the six different fine aggregates obtained from different sources. Table 1: Physical properties of fine aggregates Type of aggregate Physical properties Sand FS BG FG-T FG-U Fineness modulus 1.97 1.67 2.70 2.94 3.01 3 Relative density (g/cm ) 2.62 2.62 2.49 3.00 3.10 Water absorption (%) 0.87 1.23 ~0 ~0 ~0

Barite 2.70 4.10 1.47

2.2. Mix proportions All the mortars were proportioned with an aggregate-binder ratio of 2.5 (by volume) and water-binder ratio of 0.45. Twenty-five percent of the total binder was fly ash. The mix design parameters of the mortars were kept constant except that different types of fine aggregate were used. The details of the mix proportions are shown in Table 2.

*First author: t.ling.1@bham.ac.uk; tcling611@yahoo.com

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Table 2: Mix proportions of cement mortars Binder Mix notation Fly Cement Sand FS ash Sand mortar 456 152 1519 FS mortar 456 152 1519 BG mortar 456 152 FG-T mortar 456 152 FG-U mortar 456 152 Barite mortar 456 152 -

Fine aggregate BG 1446 FG-T 1734 FG-U 1734 Barite 2370 Water 273 273 273 273 273 273

2.3. Mortar sample preparation For each of the mix proportions, all the materials used were put into a standard rotating drum type mixer and mixed for 5 min. The freshly mixed mortar was placed into steel moulds (4040160 mm prim samples) in two layers of approximately equal depth. After each layer was filled, the mortar in the moulds was compacted by using a mechanical vibrating table. For the radiation shielding test, thin disc steel moulds with dimensions of 1001005 mm were used. After the first layer of fresh mortar was filled, a rough compaction was applied by rodding the moulds 5 times uniformly over the cross section. After the second (final) layer was placed, the moulds were placed on a mechanical vibrating table for compaction. All the prepared specimens were covered with a plastic sheet and kept in the laboratory at a temperature of 233C. After one day, the specimens were demoulded and water cured for a further 27 days at an average temperature of 253C before testing. 2.4. Hardened density and strength tests Prim samples of 4040160 mm were used for determining the hardened density (ASTM C642), flexural strength (ASTM C348) and equivalent compressive strength (ASTM C349) of the mortars. All mechanical test results reported are the averages of three measurements. 2.5. X-ray irradiation test For each mix proportion, five disc samples were used to assess the properties of radiation shielding. The x-ray radiation shielding test was performed in an x-ray laboratory designed for medical diagnostic examination. The laboratory was installed with a medium frequency x-ray unit (Toshiba, KXO-30R). Quality assurance tests for this unit were performed regularly. These tests included output reproducibility, kVp accuracy and kVp reproducibility. The results confirmed the very good performance of this x-ray source with the coefficient of variation for all these tests being less than 2%. The distance between the target of the diagnostic x-ray tube (DXB-0324CS-A) and the test samples was kept at 700 mm. The dose at a point in free air beneath the samples was measured by a 6 c.c. ionization chamber linked to a radiation monitor controller (Model 9015, Radcal Corporation). The sensor was placed 100 mm beneath the test samples. Fig. 2 shows respectively the schematic diagram and the photograph of the experimental test setup used for this study. *First author: t.ling.1@bham.ac.uk; tcling611@yahoo.com Page 4

X-ray tube

Lead collimators

X-ray beam size: (60 mm 60 mm) = 2.45 1000mm Sample

300mm 200mm Table-top 6cc Ion. Chamber (Radiation sensor)

Fig. 2. Schematic diagram of the experimental setup of x-ray radiation shielding tests

3. Results and discussion 3.1. Flexural and compressive strengths Figs. 3 and 4 present the flexural and compressive strengths of the mortars containing different types of aggregate. The strength results depended on the types of aggregate used in the mortar. The flexural and compressive strengths of the mortar prepared with the natural aggregates (sand and FS) were higher than the mortars prepared with recycled glass aggregates (BG, FG-T and FG-U). The lower strength was likely related to the smooth surface and impermeable properties of the glass aggregates, which weaken the bonds between the glass particles and the cement paste. This is consistent with the results of our previous study [14]. But all the mortars strengths were still >30 MPa. Furthermore, the mortar prepared with barite aggregate showed particularly high compressive strength of 52.4 MPa at 28 days. This may be due to the characteristic structure of barite [15].

*First author: t.ling.1@bham.ac.uk; tcling611@yahoo.com

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2 8 -d a y flex u ra l stren g th (M P a )

0 Sand mortar FS mortar B G mortar FG-T mortar FG-U mortar B arite mortar

Fig. 3. 28-day flexural strength of mortars.

60

2 8 -d a y co m p ressiv e stren g th (M P a )

50 40 30 20 10 0 Sand mortar FS mortar B G mortar FG-T mortar FG-U mortar B arite mortar

Fig. 4. 28-day compressive strength of mortars. 3.2. Hardened density The results of the hardened density of the mortars are shown in Fig. 5. As would be expected, the density of the mortars is directly related to the specific gravity of the aggregates used. The barite mortar showed the highest density amongst all the samples *First author: t.ling.1@bham.ac.uk; tcling611@yahoo.com Page 6

examined, followed by FG-U mortar, FG-T mortar, with a density of 3043 kg/m3, 2546 kg/m3 and 2472 kg/m3, respectively. This can be attributed to the high molecular weight of BaSO4 in barite and lead oxide metal contained in the CRT funnel glass, which increased the specific gravity of aggregate and consequently increased the mortar density [10]. For the mortars prepared with sand, FS and BG, the density values were quite similar due to the comparable density of the aggregates.

3300

H a rd en ed d en sity (k g /m 3 )

3100 2900 2700 2500 2300 2100 1900 1700 1500 Sand mortar FS mortar B G mortar FG-T mortar FG -U mortar B arite mortar

Fig. 5. Hardened density of mortars. 3.3. Radiation shielding properties The radiation dose detected beneath the mortars gave an indication of the effectiveness of the mortars to shield the passage of the x-ray irradiation. The lower the detected dose meant that the higher shielding capability. All the dose values reported in this study are the average values of five replicated samples. 3.3.1. Influence of aggregate type It is seen from Fig. 6 that the doses detected for the sand, FS and BG mortars were approximately the same, probably due to the similar density values of the three types of [13, 16]. To check the feasibility of using the mortars for radiological applications, their shielding capabilities are compared with conventional red brick and lightweight brick at a constant irradiation energy of 140 kVp. As can be seen in Fig. 6, the dose values detected for the mortar made with sand, FS and BG, were 50.1%, 50.9% and 40.3% higher than that obtained for conventional red brick, respectively. Unlike beverage glass, a drastic improvement in shielding was recorded when recycled CRT funnel glass (both FG-T and FG-U) was incorporated into the mortars. For instance, compared with the case of red brick, the doses detected decreased by 47.2% and 48.8% *First author: t.ling.1@bham.ac.uk; tcling611@yahoo.com Page 7

for FG-T mortar and FG-U mortar respectively. This is because the recycled funnel glass contained a high percentage of lead oxide (PbO), which made the glass cullets denser and thus enhance its ability to block x-ray radiation. It is also noted that the removal of lead on the FG-T surface through the acid treatment process had an insignificant effect on shielding ability.

3.0

2.5

D o se (m G y )

2.0

1.5 1.0

0.5

0.0 Sand mortar FS mortar B G mortar FG -T mortar FG -U mortar B arite mortar R e d brick Lightwe ight brick

Fig. 6. Dose attained beneath 5mm thick mortars. As expected, the effectiveness of the mortar as a shielding material can be enhanced significantly with the use of barite as an aggregate. The barite mortar showed the lowest detected dose value, which represented about an 88.3% and 92.2% reduction as compared to red brick and sand mortar, respectively. The results are consistent with others [1, 8]. This has proven that the barite aggregate is particularly well-suited for use in cement mortar for radiation shielding applications. 3.3.2. Influence of mortar thickness Fig. 7 shows the influence of mortar thickness on dose detected. There was a significant gain in radiation protection with an increase in thickness. For example, as the shielding thickness was increased from 5 mm to 10 mm, the dose detected for the mortars prepared with sand, FS, BG, FG-T, FG-U and barite were reduced by 34.5%, 34.8%, 34.7%, 62.4%, 58.9%, and 79.4%, respectively. But the reduction was not linear, but rather followed an exponential decreasing trend. At 15 mm thickness, non-radiation dose was detected for barite mortar and the reduction rate was seen to be greater than other tested mortars. This means that the photoelectric interaction/attenuation of barite mortar (which contains elements of high atomic number) were higher than other investigated shielding mortars, for a given thickness of sample. It *First author: t.ling.1@bham.ac.uk; tcling611@yahoo.com Page 8

can be concluded that the degree of radiation protection can be compounded with either thicker or denser shielding materials or combination of both.

5.0 4.5 4.0

Sa nd morta r FS morta r B G morta r FG-T morta r FG-U mortar B a rite morta r

D o se (m G y )

3.5 3.0 2.5 2.0 1.5 1.0 0.5 0.0 0 5 10 15 20

25

30

S a m ple s thic k ne ss (mm)

Fig. 7. Dose attained beneath the shielding mortars at different thicknesses. 3.3.3. Influence of different x-ray energy level It is well-known that the energy level used in a general radiography room is in the range 60-120 kVp [17]. Therefore, it is important to ascertain the shielding efficiency of the mortars under irradiation of x-ray energy between 40 and 140 kVp. The influence of x-ray energy levels on the shielding efficiency of 5 mm thick mortars are plotted in Fig. 8. As the irradiation energy increased, the dose detected beneath the mortars increased. The slope of the ascending curves become steeper, particularly for the mortars made with sand, FS and BG. In other words, when barite aggregate or lead-laden recycled CRT funnel glass was incorporated into the mortars, the ability of the mortars to withstand high irradiation energy exposure was much more effective than that of conventional sand mortars.

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3.0
Sand mortar FS morta r B G mortar FG-T mortar FG-U mortar B arite morta r

2.5

D o se (m G y )

2.0

1.5

1.0

0.5

0.0 0 20 40 60 80 100 120 140 160

X-ra y e ne rg y le vel (k Vp)

Fig. 8. Dose attained beneath shielding mortars at different irradiation x-ray energies. 3.3.2. Linear attenuation coefficients, tenth-value layer and half-value layer thickness The attenuation characteristics of the mortars for x-ray energy of 140 kVp were determined and are summarized in Table 3 and Fig. 9. Table 3: Attenuation characteristics of shielding mortars for x-ray energy of 140 kVp Samples Lead rubber Sand mortar FS mortar BG mortar FG-T mortar FG-U mortar Barite mortar Attenuation coefficient (mm-1) 4.010 0.069 0.069 0.069 0.167 0.171 0.284 1mm lead equivalent 1.00 57.73 58.38 58.50 24.09 23.39 14.11 Half-value layer (mm) 0.17 9.98 10.09 10.11 4.16 4.04 2.44 Tenth-value layer (mm) 0.57 33.15 33.52 33.59 13.83 13.43 8.10

The linear attenuation coefficient (LAC,) for the mortars was calculated according to the equation: Ix = I0ex, where, I0 is the dose detected without shielding, Ix is the dose detected with shielding and x is the mortar thickness. It can be clearly noticed that the LAC for the mortars prepared with sand, FS and BG were significantly lower than the mortars prepared with FG-T, FG-U and barite. *First author: t.ling.1@bham.ac.uk; tcling611@yahoo.com Page 10

Half-value layer (HVL) and tenth-value layer (TVL) are the thickness of shielding material required to attenuate the radiation by half and 90%, respectively. As can be seen in Table 3, the HVL and TVL are always inversely proportional to the LAC. The 1 mm lead equivalent values also showed a similar trend. For example, if a proactive layer with a lead equivalent of 1 mm is required, 57.7 mm of sand mortar is needed. However, using a denser shielding mortar can considerably reduce the materials to achieve the same effect. The thickness can be reduced by about 58.2%, 57.4% and 75.6% when sand mortar is replaced by FG-T, TG-U and barite mortars, respectively.

1 mm lead e quivale nt

Tenth-value la ye r (TV L) thic kne ss

H alf-value la yer (H V L) thic kne ss

70 60 50 40 30 20 10 0 Le ad S and mortar FS mortar B G mortar FG -T mortar FG -U mortar B arite mortar

Fig. 9. Radiation shielding thickness of mortars corresponding to 1 mm lead rubber. 4. Conclusion In this work, the feasibility of using different types of aggregate in cement mortar for diagnostic x-rays shielding has been demonstrated. The results show that all the studied mortars achieved a 28th day compressive strength >30MPa. The mortars prepared with barite or lead-laden recycled CRT funnel glass enhanced radiation shielding ability due to the increases in density of the mortar. The mortars, in particular the barite mortar can be used as rendering or plastering materials for medical diagnostic and CT scanner room construction. Acknowledgment The authors would like to thank the Environment and Conservation Fund and the Woo Wheelock Greed Fund, and The Hong Kong Polytechnic University for funding support.

S h ield in g th ick n ess (m m )

*First author: t.ling.1@bham.ac.uk; tcling611@yahoo.com

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References 1. Akkurt I, Basyigit C, Kilincarslan S, Mavi B, Akkurt A (2006) Radiation shielding of concretes containing different aggregates. Cem Concr Compos 28 (2): 153-157. 2. Basyigit C, Akkurt I, Altindag R, Kilincarslan S, Akkurt A, Mavi B, Karaguzel R 2006 The effect of freezingthawing (FT) cycles on the radiation shielding properties of concretes. Build Envir 41 (8): 1070-1073. 3. Gencel O, Brostow W, Ozel C, Filiz M (2010) Concretes containing hematite for use as shielding barriers. Mater Sci 16 (3): 249-256. 4. Sakr K, EL-Hakim E (2005) Effect of high temperature or fire on heavy weight concrete properties. Cem Concr Res 35 (3): 590-596. 5. Miah MI (2004) Environmental gamma dose rates and influencing factors in buildings. Build Envir 39 (7): 847-850. 6. Kharita MH, Yousef S, AlNassar M (2009) The effect of carbon powder addition on the properties of hematite radiation shielding concrete. Prog Nucl Ener 51 (2): 388392. 7. Kharita MH, Takeyeddin M, Alnassar M, Yousef S (2008) Development of special radiation shielding concretes using natural local materials and evaluation of their shielding characteristics. Prog Nucl Ener 50 (1): 33-36. 8. Sakr K (2006) Effects of silica fume and rice husk on the properties of heavy weight concrete. J Mater Civil Eng 3 (1): 367-376. 9. Akkurt I, Akyldrm H, Mavi B, Kilincarslan S, Basyigit C (2010) Radiation shielding of concrete containing zeolite. Rad Measur 45 (7): 827-830. 10. Ling TC, Poon CS (2011) Utilization of recycled glass derived from cathode ray tube glass as fine aggregate in cement mortar. J Hazard Mater 192(2): 451-456. 11. Lee G, Ling TC, Wong YL, Poon CS (2011) Effects of crushed glass cullet sizes, casting methods and pozzolanic materials on ASR of concrete blocks. Constr Build Mater 25(5): 2611-2618. 12. Ling TC, Poon CS (2012) A comparative study on the feasible use of recycled beverage and CRT funnel glass as fine aggregate in cement mortar. J Cleaner Product 29-30:46-52. 13. Ling TC, Poon CS (2012) Effects of particle size of treated CRT funnel glass on properties of cement mortar. Mater Struct, DOI: 10.1617/s11527-012-9880-8 14. Ling TC, Poon CS (2011) Properties of architectural mortar prepared with recycled glass with different particle sizes. Mater Desg 32 (5): 2675-2684. 15. Esen Y, Yilmazer B (2010) Investigation of some physical and mechanical properties of concrete produced with barite aggregate. Sci Res Essays 5 (24): 3826-333. 16. Ling TC, Poon CS, Kou SC (2011) Feasibility of using recycled glass in architectural cement mortars. Cem Concr Compos 33 (8): 848-854. 17. Okkalides D (1999) Assessment of radiology installations in Macedonia, Greece. Eur J Radiol 12 (3): 177-181.

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