Distinct effects of irradiation on the structure and chemical reactivity of silicates and carbonates

Erika Callagon la Plante; Yi Hsuan Hsiao; Isabella Pignatelli; Aditya Kumar; N. M.Anoop Krishnan; Tandré Oey; Howard Dobbs; Yingtian Yu; Bu Wang; Narayanan Neithalath; Kevin G. Field; Jacob Israelachvili; Yann Le Pape; Mathieu Bauchy; Gaurav Sant

Distinct effects of irradiation on the structure and chemical reactivity of silicates and carbonates

Erika Callagon la Plante, Yi Hsuan Hsiao, Isabella Pignatelli, Aditya Kumar, N. M.Anoop Krishnan, Tandré Oey, Howard Dobbs, Yingtian Yu, Bu Wang, Narayanan Neithalath, Kevin G. Field, Jacob Israelachvili, Yann Le Pape, Mathieu Bauchy, Gaurav Sant

Nuclear Structures and Construction

Research output: Contribution to conference › Paper › peer-review

Abstract

Concrete in nuclear power plants (NPP) is subject to sustained exposure to neutron irradiation. The interaction of neutrons with crystalline components of concrete, e.g.., the mineral aggregates, may result in its premature degradation by, for example, alkali-silica reaction leading to cracking. In this collection of studies, we investigated the effects of irradiation on the structure and reactivity of a wide variety of minerals typical of concrete aggregates. The silicates quartz (SiO₂), albite (NaAlSi₃O₈), and almandine (Fe₃Al₂(SiO₄)₃), and the carbonates calcite (CaCO₃) and dolomite (CaMg(CO₃)₂) were irradiated using Ar⁺ ions at 400 keV. Molecular dynamics simulations enabled the characterization of network rigidity of pristine and irradiated samples from the magnitudes of radial and angular bond excursions. Dissolution rates quantified using vertical scanning interferometry showed that the minerals underwent various degrees of enhancement in reactivity upon irradiation, ranging from nearly unchanged (i.e., calcite and dolomite) to a factor of 1000 (i.e., quartz). The observed increase in dissolution rates for a variety of aqueous environments depended on the nature and magnitude of the relative decrease in network rigidity upon irradiation, as well on the specific dissolution mechanism of the phase. The dominance of ionic bonding in carbonates rendered the phase resilient to irradiation, whereas the breakage of Si–O bonds in the percolated silicates albite and quartz resulted in structural disorder. In addition, the trends in reactivity alterations are consistent with the corresponding changes in density. These findings can help guide assessments of susceptibility of concrete to irradiation-induced damage and inform selections of durable aggregates.

Original language	English
Pages	582-586
Number of pages	5
State	Published - 2019
Event	19th International Conference on Environmental Degradation of Materials in Nuclear Power Systems - Water Reactors, EnvDeg 2019 - Boston, United States Duration: Aug 18 2019 → Aug 22 2019

Conference

Conference	19th International Conference on Environmental Degradation of Materials in Nuclear Power Systems - Water Reactors, EnvDeg 2019
Country/Territory	United States
City	Boston
Period	08/18/19 → 08/22/19

Funding

The authors acknowledge financial support for this research provided by: The Oak Ridge National Laboratory (ORNL) operated for the U.S. Department of Energy by UT-Battelle (LDRD Award Number: 4000132990), National Science Foundation (CMMI: 1066583 and 1235269), Department of Energy’s Nuclear Energy University Program (DOE-NEUP: DENE0008398), National Science Foundation (CAREER award: 1253269), the U.S. Department of Transportation (U.S. DOT) through the Federal Highway Administration (DTFH61-13-H-00011), and University of California, Los Angeles (UCLA). The contents of this paper reflect the views and opinions of the authors who are responsible for the accuracy of the data presented. This research was carried out in the Laboratory for the Chemistry of Construction Materials (LC2) at UCLA, Molecular Instrumentation Center (MIC), the Laboratory for the Physics of Amorphous and Inorganic Solids (PARISlab) at UCLA, the Michigan Ion Beam Laboratory (MIBL), and the Low Activation Materials Development and Analysis (LAMDA) facility of ORNL. As such, the authors gratefully acknowledge the support that has made these laboratories and their operations possible. The authors acknowledge financial support for this research provided by: The Oak Ridge National Laboratory (ORNL) operated for the U.S. Department of Energy by UT-Battelle (LDRD Award Number: 4000132990), National Science Foundation (CMMI: 1066583 and 1235269), Department of Energy?s Nuclear Energy University Program (DOE-NEUP: DENE0008398), National Science Foundation (CAREER award: 1253269), the U.S. Department of Transportation (U.S. DOT) through the Federal Highway Administration (DTFH61-13-H-00011), and University of California, Los Angeles (UCLA). The contents of this paper reflect the views and opinions of the authors who are responsible for the accuracy of the data presented. This research was carried out in the Laboratory for the Chemistry of Construction Materials (LC2) at UCLA, Molecular Instrumentation Center (MIC), the Laboratory for the Physics of Amorphous and Inorganic Solids (PARISlab) at UCLA, the Michigan Ion Beam Laboratory (MIBL), and the Low Activation Materials Development and Analysis (LAMDA) facility of ORNL. As such, the authors gratefully acknowledge the support that has made these laboratories and their operations possible.

Funders	Funder number
DOE-NEUP	1253269, DENE0008398
DOE Office of Nuclear Energy
National Science Foundation
U.S. Department of Energy
U.S. Department of Transportation
Division of Civil, Mechanical and Manufacturing Innovation	1235269, 1066583
Oak Ridge National Laboratory
Federal Highway Administration	DTFH61-13-H-00011
Nuclear Energy University Program
Laboratory Directed Research and Development	4000132990
University of California, Los Angeles
UT-Battelle

Cite this

la Plante, E. C., Hsiao, Y. H., Pignatelli, I., Kumar, A., Krishnan, N. M. A., Oey, T., Dobbs, H., Yu, Y., Wang, B., Neithalath, N., Field, K. G., Israelachvili, J., Le Pape, Y., Bauchy, M., & Sant, G. (2019). Distinct effects of irradiation on the structure and chemical reactivity of silicates and carbonates. 582-586. Paper presented at 19th International Conference on Environmental Degradation of Materials in Nuclear Power Systems - Water Reactors, EnvDeg 2019, Boston, United States.

@conference{7bdedea0f6e6469c85f098d3faaf20b6,

title = "Distinct effects of irradiation on the structure and chemical reactivity of silicates and carbonates",

abstract = "Concrete in nuclear power plants (NPP) is subject to sustained exposure to neutron irradiation. The interaction of neutrons with crystalline components of concrete, e.g.., the mineral aggregates, may result in its premature degradation by, for example, alkali-silica reaction leading to cracking. In this collection of studies, we investigated the effects of irradiation on the structure and reactivity of a wide variety of minerals typical of concrete aggregates. The silicates quartz (SiO2), albite (NaAlSi3O8), and almandine (Fe3Al2(SiO4)3), and the carbonates calcite (CaCO3) and dolomite (CaMg(CO3)2) were irradiated using Ar+ ions at 400 keV. Molecular dynamics simulations enabled the characterization of network rigidity of pristine and irradiated samples from the magnitudes of radial and angular bond excursions. Dissolution rates quantified using vertical scanning interferometry showed that the minerals underwent various degrees of enhancement in reactivity upon irradiation, ranging from nearly unchanged (i.e., calcite and dolomite) to a factor of 1000 (i.e., quartz). The observed increase in dissolution rates for a variety of aqueous environments depended on the nature and magnitude of the relative decrease in network rigidity upon irradiation, as well on the specific dissolution mechanism of the phase. The dominance of ionic bonding in carbonates rendered the phase resilient to irradiation, whereas the breakage of Si–O bonds in the percolated silicates albite and quartz resulted in structural disorder. In addition, the trends in reactivity alterations are consistent with the corresponding changes in density. These findings can help guide assessments of susceptibility of concrete to irradiation-induced damage and inform selections of durable aggregates.",

author = "{la Plante}, {Erika Callagon} and Hsiao, {Yi Hsuan} and Isabella Pignatelli and Aditya Kumar and Krishnan, {N. M.Anoop} and Tandr{\'e} Oey and Howard Dobbs and Yingtian Yu and Bu Wang and Narayanan Neithalath and Field, {Kevin G.} and Jacob Israelachvili and {Le Pape}, Yann and Mathieu Bauchy and Gaurav Sant",

note = "Publisher Copyright: {\textcopyright} 2019 19th International Conference on Environmental Degradation of Materials in Nuclear Power Systems - Water Reactors, EnvDeg. All rights reserved.; 19th International Conference on Environmental Degradation of Materials in Nuclear Power Systems - Water Reactors, EnvDeg 2019 ; Conference date: 18-08-2019 Through 22-08-2019",

year = "2019",

language = "English",

pages = "582--586",

}

la Plante, EC, Hsiao, YH, Pignatelli, I, Kumar, A, Krishnan, NMA, Oey, T, Dobbs, H, Yu, Y, Wang, B, Neithalath, N, Field, KG, Israelachvili, J, Le Pape, Y, Bauchy, M & Sant, G 2019, 'Distinct effects of irradiation on the structure and chemical reactivity of silicates and carbonates', Paper presented at 19th International Conference on Environmental Degradation of Materials in Nuclear Power Systems - Water Reactors, EnvDeg 2019, Boston, United States, 08/18/19 - 08/22/19 pp. 582-586.

Distinct effects of irradiation on the structure and chemical reactivity of silicates and carbonates. / la Plante, Erika Callagon; Hsiao, Yi Hsuan; Pignatelli, Isabella et al.
2019. 582-586 Paper presented at 19th International Conference on Environmental Degradation of Materials in Nuclear Power Systems - Water Reactors, EnvDeg 2019, Boston, United States.

Research output: Contribution to conference › Paper › peer-review

TY - CONF

T1 - Distinct effects of irradiation on the structure and chemical reactivity of silicates and carbonates

AU - la Plante, Erika Callagon

AU - Hsiao, Yi Hsuan

AU - Pignatelli, Isabella

AU - Kumar, Aditya

AU - Krishnan, N. M.Anoop

AU - Oey, Tandré

AU - Dobbs, Howard

AU - Yu, Yingtian

AU - Wang, Bu

AU - Neithalath, Narayanan

AU - Field, Kevin G.

AU - Israelachvili, Jacob

AU - Le Pape, Yann

AU - Bauchy, Mathieu

AU - Sant, Gaurav

PY - 2019

Y1 - 2019

N2 - Concrete in nuclear power plants (NPP) is subject to sustained exposure to neutron irradiation. The interaction of neutrons with crystalline components of concrete, e.g.., the mineral aggregates, may result in its premature degradation by, for example, alkali-silica reaction leading to cracking. In this collection of studies, we investigated the effects of irradiation on the structure and reactivity of a wide variety of minerals typical of concrete aggregates. The silicates quartz (SiO2), albite (NaAlSi3O8), and almandine (Fe3Al2(SiO4)3), and the carbonates calcite (CaCO3) and dolomite (CaMg(CO3)2) were irradiated using Ar+ ions at 400 keV. Molecular dynamics simulations enabled the characterization of network rigidity of pristine and irradiated samples from the magnitudes of radial and angular bond excursions. Dissolution rates quantified using vertical scanning interferometry showed that the minerals underwent various degrees of enhancement in reactivity upon irradiation, ranging from nearly unchanged (i.e., calcite and dolomite) to a factor of 1000 (i.e., quartz). The observed increase in dissolution rates for a variety of aqueous environments depended on the nature and magnitude of the relative decrease in network rigidity upon irradiation, as well on the specific dissolution mechanism of the phase. The dominance of ionic bonding in carbonates rendered the phase resilient to irradiation, whereas the breakage of Si–O bonds in the percolated silicates albite and quartz resulted in structural disorder. In addition, the trends in reactivity alterations are consistent with the corresponding changes in density. These findings can help guide assessments of susceptibility of concrete to irradiation-induced damage and inform selections of durable aggregates.

AB - Concrete in nuclear power plants (NPP) is subject to sustained exposure to neutron irradiation. The interaction of neutrons with crystalline components of concrete, e.g.., the mineral aggregates, may result in its premature degradation by, for example, alkali-silica reaction leading to cracking. In this collection of studies, we investigated the effects of irradiation on the structure and reactivity of a wide variety of minerals typical of concrete aggregates. The silicates quartz (SiO2), albite (NaAlSi3O8), and almandine (Fe3Al2(SiO4)3), and the carbonates calcite (CaCO3) and dolomite (CaMg(CO3)2) were irradiated using Ar+ ions at 400 keV. Molecular dynamics simulations enabled the characterization of network rigidity of pristine and irradiated samples from the magnitudes of radial and angular bond excursions. Dissolution rates quantified using vertical scanning interferometry showed that the minerals underwent various degrees of enhancement in reactivity upon irradiation, ranging from nearly unchanged (i.e., calcite and dolomite) to a factor of 1000 (i.e., quartz). The observed increase in dissolution rates for a variety of aqueous environments depended on the nature and magnitude of the relative decrease in network rigidity upon irradiation, as well on the specific dissolution mechanism of the phase. The dominance of ionic bonding in carbonates rendered the phase resilient to irradiation, whereas the breakage of Si–O bonds in the percolated silicates albite and quartz resulted in structural disorder. In addition, the trends in reactivity alterations are consistent with the corresponding changes in density. These findings can help guide assessments of susceptibility of concrete to irradiation-induced damage and inform selections of durable aggregates.

UR - http://www.scopus.com/inward/record.url?scp=85080033127&partnerID=8YFLogxK

M3 - Paper

AN - SCOPUS:85080033127

SP - 582

EP - 586

T2 - 19th International Conference on Environmental Degradation of Materials in Nuclear Power Systems - Water Reactors, EnvDeg 2019

Y2 - 18 August 2019 through 22 August 2019

ER -

Distinct effects of irradiation on the structure and chemical reactivity of silicates and carbonates

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