Direct Experimental Evidence for Differing Reactivity Alterations of Minerals following Irradiation: The Case of Calcite and Quartz

Isabella Pignatelli, Aditya Kumar, Kevin G. Field, Bu Wang, Yingtian Yu, Yann Le Pape, Mathieu Bauchy, Gaurav Sant

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Abstract

Concrete, used in the construction of nuclear power plants (NPPs), may be exposed to radiation emanating from the reactor core. Until recently, concrete has been assumed immune to radiation exposure. Direct evidence acquired on Ar+-ion irradiated calcite and quartz indicates, on the contrary, that, such minerals, which constitute aggregates in concrete, may be significantly altered by irradiation. More specifically, while quartz undergoes disordering of its atomic structure resulting in a near complete lack of periodicity, calcite only experiences random rotations, and distortions of its carbonate groups. As a result, irradiated quartz shows a reduction in density of around 15%, and an increase in chemical reactivity, described by its dissolution rate, similar to a glassy silica. Calcite however, shows little change in dissolution rate - although its density noted to reduce by ≈9%. These differences are correlated with the nature of bonds in these minerals, i.e., being dominantly ionic or covalent, and the rigidity of the mineral's atomic network that is characterized by the number of topological constraints (nc) that are imposed on the atoms in the network. The outcomes have major implications on the durability of concrete structural elements formed with calcite or quartz bearing aggregates in nuclear power plants.

Original languageEnglish
Article number20155
JournalScientific Reports
Volume6
DOIs
StatePublished - Jan 29 2016

Funding

The authors acknowledge financial support for this research provided by: The Oak Ridge National Laboratory operated for the U.S. Department of Energy by UT-Battelle (LDRD Award Number: 4000132990), National Science Foundation (CMMI: 1066583 and 1235269), Federal Highway Administration (DTFH61-13-H-00011) and the 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 data presented herein. This research was conducted in: Laboratory for the Chemistry of Construction Materials (LC2), the Laboratory for the Physics of AmoRphous and Inorganic Solids (PARISlab), and the Molecular Instrumentation Center (MIC) at UCLA, the Michigan Ion Beam Laboratory (MIBL) and the Low Activation Materials Development and Analysis (LAMDA) facility of Oak Ridge National Laboratory (ORNL). Support for KGF was provided by the ORNL Alvin M. Weinberg Fellowship. The authors gratefully acknowledge the support that has made these laboratories and their operations possible. This manuscript has been co-authored by UT-Battelle, LLC under Contract: DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). The authors acknowledge Prof. Jacob Israelachvili (UCSB) for stimulating and insightful discussions on the dissolution behaviors and mechanisms of silicates.

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