International Symposium on the Ageing Management & Maintenance of Nuclear Power Plants (2010) 173-182

Irradiation Effects on Concrete Structure

Osamu Kontani 1), Yoshikazu Ichikawa 1), Akihiro Ishizawa 1), Masayuki Takizawa 2) and Osamu Sato 2) 1) Kajima Corporation, Nuclear Power Department, 6-5-11 Akasaka, Minato-ku, Tokyo, 107-8348, Japan, (kontani, yichi, ishizawa-akihiro)@kajima.com 2) Mitsubishi Research Institute Inc., Science and Safety Policy Research Division Nuclear Energy Systems Group, 2-10-3 Nagatacho, Chiyoda-ku, Tokyo 100-8141, Japan, (takizawa, sato)@mri.co.jp

ABSTRACT
When the soundness of irradiated concrete in nuclear power plants operated for more than 30 years was assessed, radiation doses of 1x1020 n/cm2 for fast neutrons and 2x1010 rad (2x108 Gy) for gamma rays were adopted as reference levels of nuclear radiation. Concrete structures have been regarded to be sound as long as the radiations do not exceed the reference levels, even if the power plants are operated for more than 30 years. The reference levels were estimated from experimental data summarized by Hilsdorf [The Effects of Nuclear Radiation on the Mechanical Properties of Concrete, ACI SP-55, 1978]. However, the experimental conditions on the data were much different from irradiation conditions for concrete structures in light water reactor power plant. This paper reexamines the applicability of the reference levels to the soundness evaluation of concrete against nuclear radiations and claims that additional irradiation tests are needed for determining more reliable reference levels in assessing the soundness of irradiated concrete.

1. INTRODUCTION
In Japan, twenty nuclear power plants (NPP) have undergone an examination called PLM (Plant Life Management) by Japanese government to determine if they are sound against ageing after 30 years of operation. Three of these twenty plants have undergone PLM after 40 years of operation. Japan has now entered a period of the safety management of many aged NPP. Concrete has been widely used as a construction material for nuclear power plants, so that concrete is the subject for PLM. Two deterioration phenomena, the reductions of concrete strength and shielding ability, are chosen for the PLM examination. These reductions are induced by several deterioration factors such as heat, irradiation, neutralization, salt intrusion and so on. In the PLM assessment, the soundness against each factor is examined to show that the reductions do not take place during the plant operation. In assessing the reduction of concrete strength under nuclear radiation fields, 1x1020 n/cm2 for fast neutrons and 2x1010 rad (2x108 Gy) for gamma rays have been adopted as the reference levels of nuclear radiations. Concrete structures have been regarded to be sound as long as the radiations do not exceed the reference levels, even if the power plants are operated for more than 30 years. The reference levels were estimated from experimental data that were summarized by Hilsdorf [1]. However, the experimental conditions on the data were much different from irradiation conditions for concrete structures in light water reactor (LWR) power plant. This paper examines the applicability of the reference levels to the soundness evaluation of concrete against nuclear radiations and claims that new irradiation tests are needed for determining more reliable reference levels in assessing the soundness of irradiated concrete.

2. REFERENCE LEVELS FOR RADIATION EXPOSURE

Most experimental studies of irradiation effects on concrete were carried out in the 1960s and 1970s. It is very difficult from these studies to deduce the mechanism of concrete deterioration by nuclear radiations. Hilsdorf put the original data together to form fluence and dose vs. residual strength ratio 173

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fcu/fcuo
Fast Neutrons Elleuch Houben & Schaaf StocesThermal Neutrons Alexander Price No Information Batten Dubrovskii
Residual Strength Ratio

Aluminous Cement or 150-200 deg C

Reference Fluence 1.0x1020

Liquid Glass 500 deg C

Fluence of Neutron Radiations(n/cm2)

Figure 1 Compressive Strength of Concrete Exposed to Neutron Radiation fcu, related to Compressive Strength of Untreated Concrete, fcuo [1]
Legend symbols were changed and some notes were added to the original.

fcu/fcuo
Residual Strength Ratio

Alexander Sommers Gray Immersed in Water

Compressive Strength

Tensile Strength

Reference Dose 2.01010

Gamma Ray Dose(rad)

Figure 2 Compressive and Tensile strength of Concrete Exposed to Gamma Radiation fcu, related to Compressive Strength of Untreated Concrete, fcuo [1]
Legend symbols were changed and some notes were added to the original.

diagrams shown in Figure 1 and Figure 2 for neutrons and gamma rays, respectively. The reference levels employed so far seems to be determined from these diagrams. Experimental conditions on the data are summarized in Table 1. Concrete structures for LWR are made from Portland cement, and the temperatures are usually kept at less than 65 deg C. The experimental conditions on some of the data referred by Hilsdorf are very different from the above conditions. The following five criteria are therefore selected to evaluate the applicability of the previous data to the PLM of LWR. 1. Whether the irradiation effect is evaluated on the compressive strength, not the tensile or bending strength. 2. Whether the same materials as LWR, such as Portland cement and ordinary aggregates, are used. 3. Whether the sizes of the specimens are not too small for measuring the compressive strength. 4. Whether the irradiation temperature is not too far from the conditions of LWR, less than 65 deg C 5. Whether the fast neutrons with the energy more than 0.1 MeV are irradiated to the specimens.

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Table 1.
Author Alexander Batten
[8]

Experimental Conditions Found in Papers Referred by Hilsdorf

Cement Type Specimen Size (mm) Irradiation Conditions Temperature Neutron Energy Level & (deg C) Fluence (n/cm2)

Property Measured

Compress. Compress.

OPC OPC Liquid glass Aluminous cement OPC OPC OPC

51x51x51 51x51x203 15x15 cylinder 25x25x50 8x8x70 51x51x203 50x70 cylinder

20 to 100 Not Available 200 to 550 210 150 to 200 50 <80

[9]

Dubrovskii Elleuch

[2]

Compress. Compress. Compress.

Bending

[3] [ ]

Houben 4 [ ] Schaaf 5 Price Stoces

[6]

[10]

Comp.

Thermal Neutron 0.29x1019 to 2.3x1019 No Information 5.0x1019 No Information 2.0x1021 to 2.4x1021 Fast Neutron 2.6x1020 to 11.1x1020 Fast Neutron 3.0x1019 to 8x1019 Thermal Neutron 0.5x1019 to 7x1019 Fast Neutron 4.2x1018

OPC : Ordinary Portland cement Conditions with gray hatching are considered to be different from those for LWR.

Then, two points in Figure 1 with the fluence more than 2x1021 n/cm2 become out of these criteria. They were obtained from samples containing liquid glass and under irradiation temperatures of up to 500 deg C [2]. Several data by Elleuch [3] between 3x1019 and 1x1020 n/cm2 are also out of these criteria. They were obtained by using aluminous cement under irradiation temperatures of 210 deg C. The compressive strength measured by Houben[4]and Schaaf[5] were obtained by using a tiny sample specimens of 8x8x70mm, and no explanation was given to the test method employed. The data obtained by Price [6] were not compressive strength but bending strength. If the above data are eliminated form Figure 1, there are no data with the fluence higher than 1x1020 n/cm2, and the trend of decreasing strength with increasing fluence becomes ambiguous. The number of data that can be used for the PLM of LWR also significantly decreases in the region between 21019 and 11020 n/cm2, which decreases the reliability of the reference level for the soundness evaluation. The situation is similar for the evaluation of the reference level for gamma irradiation. The data in Figure 2 by Sommers[7] were obtained by irradiating the samples in deionized water. Since severe corrosion was observed on the surfaces of the samples, the author attributed the reduction of the strength not by the irradiation but by the corrosion due to the deionized water. The data by Gray are not for compressive strength but for tensile strength. Elimination of these data leaves only one point on Figure 2, so that no discussion can be made on the relationships between gamma ray dose and the residual strength. These evidences indicate that additional new data are necessary for evaluating the availability of the reference levels. The new experiments should be designed for clarifying the mechanism of concrete deterioration by nuclear radiations, which necessitate knowledge on concrete and radiation sciences.

3. STRUCTURES OF CEMENT PAST AND AGGREGATE

Concrete primarily consists of water, cement and aggregate. As water reacts with cement to form hydration products (cement paste), concrete gradually develops its strength. The behaviors of cement paste and aggregate are known to differ under irradiation conditions: cement paste tends to contract slightly and aggregates tend to expand. The behavior of concrete, the heterogeneous mixture of cement past and aggregates, depends on the kind of aggregates in the concrete. For estimating appropriate reference levels, 175

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it is therefore necessary to understand the radiation effect separately on cement past and aggregates, and then to understand interactions between irradiated cement and aggregates. In this section, fundamental knowledge for understanding the radiation effect on cement paste, aggregate, and concrete will be mentioned for designing new experiments necessary for understanding the mechanism of concrete deterioration by nuclear radiations and for evaluating the availability of the reference levels. 3.1 Structure of Cement Paste Since the specific surface area is considered to be 200m2 per 1g of hardened cement paste [11], cement paste is often expressed by layered models shown in Figure 3 [12]. The spacing of the layers would be of nanometer scale. Fully hydrated cement paste contains pores comprising 26% of its volume [12]. A large amount of water exists in cement paste in different states. It can be divided into three categories based on how strongly it is bound to the hydration products as shown in Figure 4 [11]. Free water exists in capillary pores and behaves like bulk water. Gel water is absorbed (physically bound) on the surface of hydration products. During drying at 105 deg C (oven drying), gel water and capillary water can be released. Chemically bound water is strongly fixed to hydration products, and will be retained in the hydration products even after oven drying. Water in cement paste can be classified in different ways as evaporable or non-evaporable. The former is released from hardened cement paste upon oven drying. The latter is retained in paste even after oven drying. For simplicity, it is assumed that evaporable water consists of gel water and free water and that non-evaporable water corresponds to chemically bound water. The structural characteristics of cement paste are summarized in Table 2.

Figure 3.

Various structural models of calcium silica hydrate (C-S-H) in cement paste [12]
Free Water Adsorbed Water Chemically Bound WaterCSH, CH

105

Figure 4. TG and DTA curves for a fully reacted C3S paste [11]
(Some notes were added to the original.)

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3.2 Structure of Aggregates Unlike cement paste, aggregates are usually well-crystallized minerals. A large part of the earth's surface consists of SiO2 and Al2O3. Aggregates contain evaporable water as well as non-evaporable water, though the total amount is much less than that in cement paste. Evaporable water in aggregates is called absorbed water. The absorption factor of coarse aggregates used in NPPs would be less than 2.5%. Non-evaporable water in aggregates is called water of crystallization. The amount of the water of crystallization is about 0.5% to 1.5% [13]. The structural characteristics of aggregates are summarized in Table 2 together with those of cement past. Table 2 Structural Characteristics of Cement Paste and Aggregates State of Water Phase State of Solid Phase - Contains a large amount of water in - Modeled by layered structure various states. (Water content of concrete is - Porous materials (pore volume=26% [12]) around 7% of mass.) - Main components of cement paste - Classification of water - CSH (Calcium Silicate Hydrate) - Evaporable Water - CH (Calcium Hydroxide) - Free water (Capillary water) - AFt (Ettringite) - Adsorbed water (Gel water) - AFm (Monosulfoaluminate) - Non-evaporable water - CSH is responsible for the strength of - Chemically bound water cement paste. - The amount is much less than that in cement paste. - Classification of Water - Evaporable Water - Absorbed water (1-2.5%) - Non-evaporable Water - Crystal water (0.5-1.5%) - Most aggregates are well-crystallized and denser than cement paste.

Component

Cement Paste

Aggregate

4. INTERACTION BETWEEN RADIATION AND MATERIALS

4.1 Interaction between Gamma Rays and Materials There are three typical interactions between gamma rays and materials, as shown in Figure 5. Gamma rays collide with orbital electrons, one orbital electron is ejected and then the gamma ray disappears. This phenomenon is called photoelectric effects. When the gamma rays energy is much greater than the binding energy of electrons, gamma rays collide with electrons to eject the electrons and loose a part of the energies to change the travelling directions. This is called Compton scattering. When the energy of gamma rays is greater than 1.02MeV, they disappear around atomic nuclei and a pair of electron and positron is produced. This is called pair production. The ejected or produced electrons collide with materials to eject electrons, so that the number of ejected electrons (secondary electrons) continuously increases until the energies of the secondary electrons become lower than the ionization energies of the materials. Since the mass of secondary electrons is very low, they do not directly eject atoms composing the materials. Gamma rays have therefore very little effect on the solid materials composed of rather isotropic ionic and metallic bonds. On the other hand, gamma rays affect the materials through electronic excitations. Collision of the secondary electrons with materials causes electronic excitations. The excited states loose their excess electronic energies to the vibrational energies of atoms composing the materials, which results in the destruction of anisotropic chemical bonds such as covalent bond. Siliceous minerals may also be 177

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decomposed by gamma-irradiation, because Si-O bond is considered to be a covalent bond [14]. Water, a main component of concrete is thus expected to be decomposed by gamma rays to convert to hydrogen, oxygen and hydrogen peroxide [15]. Since water contents are much greater in cement paste than in aggregates, it is considered that gamma rays have more influence on cement paste than on aggregates. Gamma rays from nuclear reactors have their energy from 100keV to 10 MeV. Figure 6 shows which interaction is dominant in accordance with gamma ray energy and atomic number. Because of the atomic numbers usually found in cement paste and aggregates, gamma rays primarily decay by Compton scattering. The interactions of gamma rays on cement paste and aggregates are summarized in Table 3.
Compton Scattering Gamma Ray

Gamma Ray

Electron ejected

Electron ejected Gamma Ray

Electron ejected

Photoelectric Effect

Gamma Ray scattered Nucleus Electron

Pair Production

Positron ejected

Figure 5. Schematic Representation of Interactions between Gamma Rays and Atoms.

100

Atomic #

Photoelectric Effect

Pair Production

50 Compton Scattering 0. 1 1 10

0 0.01

Energy
100Mev

Figure 6

Interactions between Gamma Ray and Atoms

Table 3 Interactions of Gamma Rays on Cement Paste and Aggregates Water Phase Solid Phase -Water may be decomposed by radiolysis to -SiO bond of calcium -Electrons are generate hydrogen and hydrogen peroxide which silicate hydrate in ejected by in turn decomposes into water and oxygen. cement paste may be scattering of -Gamma heating may cause additional hydration slightly decomposed gamma rays and of unhydrated cement and transformation of due to the covalent collide with the hydrated cement. nature of the bond. solid phases of -Hydrogen peroxide generated in radiolysis cement paste or process may react with cement paste. aggregates. -Siliceous aggregate may be slightly decomposed.

Cement Paste

-Small amount of water may be released by the radiolysis in the form of hydrogen and oxygen Aggregate gasses as well as by gamma heating in the form of vapor.

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4.2 Interaction between Neutron and Materials Interactions between neutron and materials can be broadly classified into two categories, scattering and absorption. The two types of scattering are shown in Figure 7. When a fast neutron collides with a heavier atomic nucleus, the neutron loses its energy to become an intermediate neutron by releasing a neutron and the extra energy as scattering gamma rays, which is called inelastic scattering. When the intermediate neutron collides with a lighter nucleus such as H, C or O, a neutron is ejected and the traveling directions of neutron and nucleus are changed. This phenomenon is called elastic scattering and the total kinetic energy of the system is preserved. These neutron scatterings accompany the dislocation of atoms from the original positions. The intermediate neutrons reduce their energy to become thermal neutrons by hundreds of elastic scatterings. Once neutrons become thermal neutrons, their energy levels are not sufficient to eject neutrons from atomic nuclei. The reference level of neutrons is expressed by a fluence of fast neutrons having energy of more than 0.1MeV. Since concrete contains heavier nuclei and lighter nuclei as well, the fast neutrons reduce their energy by inelastic scattering to become intermediate neutrons and the intermediate neutrons reduce their energy by elastic scattering to become thermal neutrons. When neutrons with higher energy collide with atomic nuclei, atoms are ejected and lattice defects are created by inelastic and elastic scattering. The interactions of neutrons on cement paste and aggregates are summarized in Table 4. Neutrons have influences on the solid phase by kicking out atoms from their original locations. There are papers showing that neutrons have significant effects on aggregates. Since aggregates are dense and well-crystallized materials, when neutrons collide with crystal lattice, lattice constant is increased, defects are accumulated and volume expansion occur. There are a few test results [16] of neutron irradiation on cement paste showing that cement paste samples suffered no damage from their appearance. Although dislocation of atoms in solid cement particles may take place, the lattice defect by the distortion may not be accumulated and the deformation of the paste may be negligible due to the porosity of the paste and the fineness of the cement particles.
after collision

Inelastic Scattering before collision

Scattering Gamma Ray

Elastic Scattering before collision before collision

after collision

before collision

after collision

after collision

: Nucleus

: Neutron

Figure 7. Schematic Representation of Neutron Scattering Table 4. Interactions of Neutrons on Cement Paste and Aggregates Water Phase Solid Phase - Molecular products from -Although dislocation of atoms in solid cement particles water may be the same as may take place, the lattice defect by the distortion may those for gamma rays, but the not be accumulated and the deformation of the paste may yields are different due to the be negligible due to the porosity of the past and the difference of LET. fineness of the cement particles. - Interaction with water is the same as that in cement paste. - Lattice constants are increased due to the dislocation of atoms, and lattice defects are accumulated [11].

Cement Paste

Aggregate

LETLinear Energy Transfer

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5. MECHANISM OF CONCRETE DETERIORATION

As already mentioned, nuclear radiation causes expansion of aggregates and slight shrinkage of cement paste. Concrete, the mixture of cement paste and aggregates, expands by the irradiation and its expansion is usually larger than the volume-averaged expansion of the aggregate and cement paste, which suggests the formation of crack around the aggregate. The expansion of concrete depends on aggregates in concrete. Concrete with siliceous aggregate shows severe expansion, even if the expansion of aggregate alone is the same as that of non siliceous one, but the mechanism causing the difference is not understood very well. Table 5 summarizes deterioration of concrete due to nuclear radiation. Table 5. Deterioration of Concrete due to Nuclear Radiation Water Phase - Dying of cement paste reduces its stiffness. Drying of cement paste produces micro cracks to reduce its strength or increases surface energy of cement paste to increase strength [17]. - Additional hydration may increase the stiffness and the strength of concrete. -Hydrogen peroxide generated in radiolysis process may react with cement paste. -Neutrons have some effects on water phase of cement paste. Solid Phase - Neutrons may have some effects on solid phases of cement paste, but the details are not understood very well. - Volume expansions of aggregates may introduce micro cracking in cement paste and decrease stiffness and strength of concrete, but the details are not understood very well. - Concrete containing siliceous aggregates seems to crack more severely than non siliceous aggregate even if the expansions of aggregate alone are the same, but the mechanism causing the difference is not understood.

6. NEEDS FOR IRRADIATION TESTS

Since the reference levels are set at 2x1010 rad for gamma rays and at 1x1020 n/cm2 for fast neutrons, it is necessary to separately understand the effects of gamma rays and neutrons on concrete. Gamma ray irradiation tests can easily be done using gamma ray radiation sources, though very limited information is available on gamma ray effects on concrete compared with neutron effects. On the other hand, it is impossible to perform irradiation tests of neutron only, since neutron irradiation is always accompanied by gamma rays. It is therefore preferable to perform gamma ray irradiation tests before neutron irradiation tests and the information obtained will be leveraged for understanding the neutron effects on concrete. Under high temperature conditions, water in cement paste will be released in the form of vapor. Under radiation conditions, water will be released by gamma heating in the form of vapor and by radiation decomposition in the form of hydrogen and oxygen gases. The relationships of temperature vs. weight loss in an ordinary Portland cement paste sample are shown in Figure 4. Based on Figure 4, once we know the temperature of the cement paste samples, we can estimate what kind of water and how much water will be released from the samples. However, we have

Water Retained

Water Vapor Release due to Heat Water Release due to Radiolysis

What is left in cement paste? Gamma Ray Dose

Figure 8. Gamma Ray Dose vs. Water Retained in Concrete. 180

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information on what kind of water and how much water will be released from the samples by nuclear radiation. It is therefore necessary to obtain the relation between radiation dose and water retention in concrete as exemplified with Figure 8. Such a figure should be made between the dose and the compressive strength. These figures should also be made for fast neutrons.

7. CONCLUSIONS
(1) Technical information necessary for determining appropriate reference levels of nuclear radiation for assessing the soundness of concrete structures under irradiation fields is found to be very limited and is needs to be obtained by carrying out additional experiments. (2) Interactions between radiation and concrete are investigated, and it is noticed that neutrons and gamma rays have different effects on cement paste and aggregates in concrete. (3) The deterioration mechanisms of concrete are suspected based on interactions between radiation and concrete.

Acknowledgements. The studies were performed as a part of the project on Enhancement of Ageing Management and Maintenance of Nuclear Power Stations sponsored by the Nuclear and Industrial Safety Agency (NISA). We would like to express our deep appreciation to NISA for its sponsorship and acceptance of publication of the results.

REFERENCES
[1] [2] Hilsdorf, H. K. et al., The Effects of Nuclear Radiation on the Mechanical Properties of Concrete, ACI SP-55, 1978 Dubrovskii, V. B.; Ibragimov, Sh. Sh.; Ladygin, A. Ya. and Pergamenshckik, B. K., "The Effect of Neutron Irradiation on Certain Properties of Refractory Concretes", Atomnaya Energiya 21 , pp.108-112, 1966. Elleuch, M. R.; Dubois, F. and Rappenau, J., "Effects of Neutron Radiation on Special Concretes and their Components", American Concrete Institute, Special Publication SP-34, pp. 1071-1108, 1972. Houben, J. A., "De Bestraling van Mortelproefstukken", (Radiation of mortar specimens), Commission of the European Communities, Brussel, pp. 170-178, 1969. Van der Schaaf, C. F., "Invloed van Bestraling en Verhitting op de Sterkte van Mortels en Beton", Commission of the European Communities, Brussel, pp. 179-183, 1969. Price, B. T.; Horton, C. C. and Spinney, K. T., "Radiation Shielding", International Series of Monograph on Nuclear Energy, Pergamon Press, New York, London, Paris, pp.276-278, 1957. Sommers, J. F., Gamma Radiation Damage of Structural Concrete Immersed in Water, Health Physics, Pergamon Press, Vol. 16, pp. 503-508, 1969. Alexander, S. C., "Effects of Irradiation on Concrete, Final Results", Atomic Energy Research Establishment, Harwell, 34 pp., 1963. Batten, A. W. Ch., "Effect of Irradiation on the Strength of Concrete", Atomic Energy Research Establishment, Harwell, 13 pp., 1960. Stoces, B., Otopal, P., Juricka, V. and Gabriel, J., "The Effect of Radiation on the Mechanical Properties of Concrete", Ceskoslovenska Akademie, Translated from the Czech; Oak Ridge National Laboratory, Purchase Order: 34B-83481, Letter Release No.: T81, STS No.: 10487. Taylor, H. F. W., Cement Chemistry, Academic Press, 1990 Mindess, S. and Young, J. F., Concrete, Prentice-Hall, 1981 Kontani, O. et al., Study on Measuring Method of Chemically Bound Water Contents in Concrete, 181

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Japan Concrete Institute, Proceeding of Annual ConventionVol.29No.1pp.693-698, 2007 (written in Japanese) Kaplan, M. F., Concrete Radiation Shielding, Longman Scientific & Technical, 1989 Bouniol, P. and Aspart, A., Disappearance of Oxygen in Concrete under Irradiation : The role of Peroxides in Radiolysis, Cement and concrete research, Vol.28, No.11, pp.1669-1681, 1998 Kelly, B. T., and Davisson, T., The effects of reactor radiation on concrete, 2nd Conference on Prestressed Concrete Pressure Vessels and Their Insulation, London, 1969, p. 237 (1969) Hori, M., Strength of Hardened Cement Paste in terms of Surface Energy, Journal of the Ceramic Association, Japan 70(799), pp. 54-59, 1962 (written in Japanese)

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