Ultra-high gamma irradiation of calcium silicate hydrates: Impact on mechanical properties, nanostructure, and atomic environments

Aniruddha Baral; Elena Tajuelo Rodriguez; William A. Hunnicutt; Ercan Cakmak; Hongbin Sun; Jan Ilavsky; Yann Le Pape; Thomas M. Rosseel; Nishant Garg

doi:10.1016/j.cemconres.2022.106855

Ultra-high gamma irradiation of calcium silicate hydrates: Impact on mechanical properties, nanostructure, and atomic environments

Aniruddha Baral, Elena Tajuelo Rodriguez, William A. Hunnicutt, Ercan Cakmak, Hongbin Sun, Jan Ilavsky, Yann Le Pape, Thomas M. Rosseel, Nishant Garg

Research output: Contribution to journal › Article › peer-review

10 Scopus citations

Abstract

The concrete biological shield in a nuclear power plant receives ~100–200 MGy gamma dosage during an 80-year design life. However, precise changes in the mechanical properties and atomic environments of C-S-H at ultrahigh irradiation dosages have not been systematically documented. Here, we report that irradiation decreases C-S-H basal spacing (~ 0.6 ± 0.1 Å for 189 MGy) and increases its Young's modulus, which is attributed to the lower basal spacing as the nano porosity potentially increased and microporosity remained unchanged. Irradiation also decreased the molecular water content and increased hydroxyl groups in C-S-H, showing that interlayer water removal reduces the basal spacing. Finally, ¹H and ²⁹Si NMR results indicate some disorder in the local proton CaO-H species and slight depolymerization of the silicate structure. Together, these results indicate that the C-S-H gel stiffens upon ultrahigh gamma irradiation dosage, a finding which concerns long-term nuclear power plants operations worldwide.

Original language	English
Article number	106855
Journal	Cement and Concrete Research
Volume	158
DOIs	https://doi.org/10.1016/j.cemconres.2022.106855
State	Published - Aug 2022

Funding

This work was supported by the US Department of Energy's (DOE's) Office of Nuclear Energy, Light Water Reactor Sustainability Program, by an appointment to the ORNL Advanced Short-Term Research Opportunity program, which is sponsored by DOE and administered by the Oak Ridge Institute for Science and Education , and by DOE's Office of Nuclear Energy under DOE Idaho Operations Office Contract DE-AC07-051D14517 as part of a Nuclear Science User Facilities experiment. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Additional thanks are due to Dr. Andre Sutrisno of the School of Chemical Sciences at the University of Illinois at Urbana-Champaign for assistance with the NMR experiments; Maryla Wasiolek and Donald J. Hanson for irradiating part of the samples at SNL's GIF and providing temperature history, dose calculations, and photos of the irradiator setup; Zachary Burns for irradiation capsule fabrication, Caleb Clement for assisting with sample synthesis, and Paula Bran Anleu for helping with (U)SAXS measurements.

Funders	Funder number
DOE's Office of Nuclear Energy	DE-AC07-051D14517
Nuclear Energy, Light Water Reactor Sustainability Program
U.S. Department of Energy
Office of Science
Argonne National Laboratory	DE-AC02-06CH11357
Oak Ridge National Laboratory
Oak Ridge Institute for Science and Education

Keywords

Basal spacing
Calcium silicate hydrate
Gamma irradiation
H NMR
Nanoindentation
Si NMR

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10.1016/j.cemconres.2022.106855

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title = "Ultra-high gamma irradiation of calcium silicate hydrates: Impact on mechanical properties, nanostructure, and atomic environments",

abstract = "The concrete biological shield in a nuclear power plant receives ~100–200 MGy gamma dosage during an 80-year design life. However, precise changes in the mechanical properties and atomic environments of C-S-H at ultrahigh irradiation dosages have not been systematically documented. Here, we report that irradiation decreases C-S-H basal spacing (~ 0.6 ± 0.1 {\AA} for 189 MGy) and increases its Young's modulus, which is attributed to the lower basal spacing as the nano porosity potentially increased and microporosity remained unchanged. Irradiation also decreased the molecular water content and increased hydroxyl groups in C-S-H, showing that interlayer water removal reduces the basal spacing. Finally, 1H and 29Si NMR results indicate some disorder in the local proton CaO-H species and slight depolymerization of the silicate structure. Together, these results indicate that the C-S-H gel stiffens upon ultrahigh gamma irradiation dosage, a finding which concerns long-term nuclear power plants operations worldwide.",

keywords = "Basal spacing, Calcium silicate hydrate, Gamma irradiation, H NMR, Nanoindentation, Si NMR",

author = "Aniruddha Baral and Rodriguez, {Elena Tajuelo} and Hunnicutt, {William A.} and Ercan Cakmak and Hongbin Sun and Jan Ilavsky and {Le Pape}, Yann and Rosseel, {Thomas M.} and Nishant Garg",

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year = "2022",

month = aug,

doi = "10.1016/j.cemconres.2022.106855",

language = "English",

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T2 - Impact on mechanical properties, nanostructure, and atomic environments

AU - Baral, Aniruddha

AU - Rodriguez, Elena Tajuelo

AU - Hunnicutt, William A.

AU - Cakmak, Ercan

AU - Sun, Hongbin

AU - Ilavsky, Jan

AU - Le Pape, Yann

AU - Rosseel, Thomas M.

AU - Garg, Nishant

PY - 2022/8

Y1 - 2022/8

N2 - The concrete biological shield in a nuclear power plant receives ~100–200 MGy gamma dosage during an 80-year design life. However, precise changes in the mechanical properties and atomic environments of C-S-H at ultrahigh irradiation dosages have not been systematically documented. Here, we report that irradiation decreases C-S-H basal spacing (~ 0.6 ± 0.1 Å for 189 MGy) and increases its Young's modulus, which is attributed to the lower basal spacing as the nano porosity potentially increased and microporosity remained unchanged. Irradiation also decreased the molecular water content and increased hydroxyl groups in C-S-H, showing that interlayer water removal reduces the basal spacing. Finally, 1H and 29Si NMR results indicate some disorder in the local proton CaO-H species and slight depolymerization of the silicate structure. Together, these results indicate that the C-S-H gel stiffens upon ultrahigh gamma irradiation dosage, a finding which concerns long-term nuclear power plants operations worldwide.

AB - The concrete biological shield in a nuclear power plant receives ~100–200 MGy gamma dosage during an 80-year design life. However, precise changes in the mechanical properties and atomic environments of C-S-H at ultrahigh irradiation dosages have not been systematically documented. Here, we report that irradiation decreases C-S-H basal spacing (~ 0.6 ± 0.1 Å for 189 MGy) and increases its Young's modulus, which is attributed to the lower basal spacing as the nano porosity potentially increased and microporosity remained unchanged. Irradiation also decreased the molecular water content and increased hydroxyl groups in C-S-H, showing that interlayer water removal reduces the basal spacing. Finally, 1H and 29Si NMR results indicate some disorder in the local proton CaO-H species and slight depolymerization of the silicate structure. Together, these results indicate that the C-S-H gel stiffens upon ultrahigh gamma irradiation dosage, a finding which concerns long-term nuclear power plants operations worldwide.

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KW - Calcium silicate hydrate

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KW - H NMR

KW - Nanoindentation

KW - Si NMR

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Ultra-high gamma irradiation of calcium silicate hydrates: Impact on mechanical properties, nanostructure, and atomic environments

Abstract

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Keywords

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