Changes in mechanical and chemical-structural properties of gamma irradiated calcium silicate hydrates to an absorbed dose of 200 MGy with respect to pristine samples

Principal Investigator
Name:
Nishant Garg
Email:
[email protected]
Phone:
(208) 526-6918
Team Members:
Name: Institution: Expertise: Status:
Elena Tajuelo Rodriguez Oak Ridge National Laboratory TEM, nanoindentation, cement, concrete, gamma irradiation, nuclear magnetic resonance Post Doc
Yann Le Pape Oak ridge National Laboratory Civil engineering materials and structures Other
Aniruddah Baral University of Illinois at Urbana-Champaign Construction Materials, Electron Microscopy, Microstructure Determination, Construction Materials Characterization, Advanced Cement Chemistry Graduate Student
Experiment Details:
Experiment Title:
Changes in mechanical and chemical-structural properties of gamma irradiated calcium silicate hydrates to an absorbed dose of 200 MGy with respect to pristine samples)
Hypothesis:
Calcium silicate hydrates subjected to gamma irradiation may suffer dehydration due to hydrolysis. This can cause a decrease in viscous properties of the material decreasing its creep response. In this proposal, the drop of the viscous response of C-S-H with a high level of gamma dose (200 MGy) will be tested for the first time. Both stress relaxation and creep will be examined with nanoindentation and responses from irradiated and control samples will be compared. Morphological and chemical-str
Work Description:
In this project we will study the viscoelastic properties and changes in chemical structure and morphology of gamma-irradiated synthetic calcium silicate hydrates. Specifically, nanoindentation, XRD and TEM will be carried out on these samples. The samples were irradiated at the Co60 gamma irradiator at the GIF facility at SNL to reach 200 MGy. This irradiator has an available dose rate of 30 Gy/s and 3 months are needed to reach the desired dose. The samples were irradiated in a sealed container and the temperature was controlled below 65°C by directing compressed air to the container. Control samples that are pristine, and from the same synthesis batch, will also be analyzed for comparison with the irradiated samples.
Project Summary
The proposed project objectives are to study the changes in viscoelastic behavior, chemical structure and morphology of calcium silicate hydrates after a gamma dose of 200 MGy. Calcium silicate hydrates are considered the glue of cement and hence are important for the stability of the concrete bio-shield in nuclear power plants. The impact of high gamma doses on the viscoelastic properties of calcium silicate hydrates is not fully understood. Results from previous experiments with samples irradiated to 2.24 MGy indicate that there may be a creep reduction with gamma irradiation. The proposed experiment will be a first of its kind to study the impact of a high gamma dose (200 MGy) to inform models that predict the degradation of cement and concrete with irradiation. Since creep has been proven to delay the onset of irradiation damage, a reduction in creep will certainly impact the level of predicted damage. The outcome of the experiments is mainly the production of stress relaxation and creep curves after irradiation, accompanied by the study of chemical-structural properties to understand the factors that may drive the changes in viscous response, such as the loss of water from the interlayer and/or the precipitation of pseudomorphs. The chemical-structural changes will be studied with X-ray diffraction. Morphology and compositional changes will be examined with TEM. Viscoelastic properties will be obtained through stress relaxation and creep nanoindentation experiments. The main goal is to inform irradiation damage predictive models to support the license renewal of the light water reactor US fleet to 80 years of operation. The samples will be available at the end of January, and the experiments will be finished in 3 sessions of 5 days each during April, May and June.
Relevance
The proposed research advances DOE’s Office of Nuclear Energy mission to meet the nation’s energy, environmental, and national security needs, since it will produce data to understand irradiation degradation mechanisms in the concrete biological shield of LWRs. This research also supports the aim of the DOE NE Light Water Reactor Sustainability Program’s (LWRS) objective to support the U.S. Nuclear Commercial Fleet Second License Renewal (SLR) up to 80 years of safe and economically viable operation. Therefore, it is tied to the NE objective of enhancing the long-term viability and competitiveness of the existing U.S. reactor fleet. The jointly-sponsored NRC-DOE Expanded Materials Degradation Analysis demonstrated the need to address urgently the effects of radiation on concrete. Among the various aspects requiring attention, the effects of gamma irradiation on the constituents of the hardened cement paste are poorly understood. The effects of the expected radiation dose at the planned extended life cycle (approx. Gamma dose of 100-200 MGy) on mechanical properties of cement and concrete in the biological shield need to be predicted to ensure the materials will remain operative and safe. This project will complement previous data sets obtained through the NSUF RTE framework to understand the effect of a medium gamma dose on the order of 2.24 MGy on calcium silicate hydrates (C-S-H), by producing data sets for a much higher dose (200 MGy). Calcium silicate hydrates constitute the major part of the volume of cement paste and are the phases that provide strength to cement. Hence, it is important to understand how radiation affects the chemical stability, morphology and mechanical properties of these phases. Viscoelasticity is a crucial property of C-S-H to relax stresses that occur due to a combination of radiation shrinkage of cement paste and radiation induced volumetric expansion of the aggregates, and therefore limits damage propagation in concrete. The results of this research will then serve to inform models to predict irradiation damage in concrete, in particular, to take into account possible radiation induced changes in viscoelastic properties of the cement paste.
Book / Journal Publications

"Examination of gamma irradiated C-S-H. Part I: Chemical-structural properties" William Hunnicutt, Elena Tajuelo Rodriguez, Paramita Mondal, Yann Le Pape, Journal of the American Ceramic Society 2019 Link

"Ultra-high gamma irradiation of calcium silicate hydrates: Impact on mechanical properties, nanostructure, and atomic environments" Elena Tajuelo Rodriguez, Cement and Concrete Research 158 2022 106855 Link

Conference Publications

"Effect of gamma irradiation on creep properties of cement paste analogues" Elena Tajuelo Rodriguez, 19th International Conference on Environmental Degradation of Materials in Nuclear Power Systems – Water Reactors August 18-22, (2019)

"The effect of gamma irradiation on C-S-H" Elena Tajuelo Rodriguez, ICIC Virtual Workshop on Effects of gamma irradiation of cement systems November 20-20, (2020)

"What does irradiation do to concrete? Insights on effects at the paste and aggregate levels" Elena Tajuelo Rodriguez, EMI May 31-3, (2022)

"Irradiation impact in concrete: Gamma effects on cement paste constituents (calcium silicate hydrates) and neutron effects on minerals present in aggregates" Elena Tajuelo Rodriguez, Goldschmidt July 10-16, (2022)