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Title: Effects of Irradiation on Albite’s Chemical Durability

Abstract

Albite (NaAlSi3O8), a framework silicate of the plagioclase feldspar family and a common constituent of felsic rocks, is often present in the siliceous mineral aggregates that compose concrete. When exposed to radiation (e.g., in the form of neutrons) in nuclear power plants, the crystal structure of albite can undergo significant alterations. These alterations may degrade its chemical durability. Indeed, careful examinations of Ar+-implanted albite carried out using Fourier transform infrared spectroscopy (FTIR) and molecular dynamics simulations show that albite’s crystal structure, upon irradiation, undergoes progressive disordering, resulting in an expansion in its molar volume (i.e., a reduction of density) and a reduction in the connectivity of its atomic network. This loss of network connectivity (i.e., rigidity) results in an enhancement of the aqueous dissolution rate of albite—measured using vertical scanning interferometry (VSI) in alkaline environments—by a factor of 20. This enhancement in the dissolution rate (i.e., reduction in chemical durability) of albite following irradiation has significant impacts on the durability of felsic rocks and of concrete containing them upon their exposure to radiation in nuclear power plant (NPP) environments.

Authors:
; ORCiD logo; ORCiD logo;  [1];  [2]; ;
  1. Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  2. School of Sustainable Engineering and the Built Environment, Arizona State University, Tempe, Arizona 85287, United States
Publication Date:
Research Org.:
Univ. of California, Los Angeles, CA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE); National Science Foundation (NSF)
OSTI Identifier:
1396932
Alternate Identifier(s):
OSTI ID: 1507568; OSTI ID: 1784213
Grant/Contract Number:  
NE0008398; 1253269; AC05-00OR22725
Resource Type:
Published Article
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Volume: 121 Journal Issue: 41; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES

Citation Formats

Hsiao, Yi-Hsuan, La Plante, Erika Callagon, Krishnan, N. M. Anoop, Le Pape, Yann, Neithalath, Narayanan, Bauchy, Mathieu, and Sant, Gaurav. Effects of Irradiation on Albite’s Chemical Durability. United States: N. p., 2017. Web. doi:10.1021/acs.jpca.7b05098.
Hsiao, Yi-Hsuan, La Plante, Erika Callagon, Krishnan, N. M. Anoop, Le Pape, Yann, Neithalath, Narayanan, Bauchy, Mathieu, & Sant, Gaurav. Effects of Irradiation on Albite’s Chemical Durability. United States. https://doi.org/10.1021/acs.jpca.7b05098
Hsiao, Yi-Hsuan, La Plante, Erika Callagon, Krishnan, N. M. Anoop, Le Pape, Yann, Neithalath, Narayanan, Bauchy, Mathieu, and Sant, Gaurav. Sat . "Effects of Irradiation on Albite’s Chemical Durability". United States. https://doi.org/10.1021/acs.jpca.7b05098.
@article{osti_1396932,
title = {Effects of Irradiation on Albite’s Chemical Durability},
author = {Hsiao, Yi-Hsuan and La Plante, Erika Callagon and Krishnan, N. M. Anoop and Le Pape, Yann and Neithalath, Narayanan and Bauchy, Mathieu and Sant, Gaurav},
abstractNote = {Albite (NaAlSi3O8), a framework silicate of the plagioclase feldspar family and a common constituent of felsic rocks, is often present in the siliceous mineral aggregates that compose concrete. When exposed to radiation (e.g., in the form of neutrons) in nuclear power plants, the crystal structure of albite can undergo significant alterations. These alterations may degrade its chemical durability. Indeed, careful examinations of Ar+-implanted albite carried out using Fourier transform infrared spectroscopy (FTIR) and molecular dynamics simulations show that albite’s crystal structure, upon irradiation, undergoes progressive disordering, resulting in an expansion in its molar volume (i.e., a reduction of density) and a reduction in the connectivity of its atomic network. This loss of network connectivity (i.e., rigidity) results in an enhancement of the aqueous dissolution rate of albite—measured using vertical scanning interferometry (VSI) in alkaline environments—by a factor of 20. This enhancement in the dissolution rate (i.e., reduction in chemical durability) of albite following irradiation has significant impacts on the durability of felsic rocks and of concrete containing them upon their exposure to radiation in nuclear power plant (NPP) environments.},
doi = {10.1021/acs.jpca.7b05098},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 41,
volume = 121,
place = {United States},
year = {Sat Sep 23 00:00:00 EDT 2017},
month = {Sat Sep 23 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.jpca.7b05098

Citation Metrics:
Cited by: 32 works
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Figures / Tables:

Figure 1 Figure 1: Crystal structure of albite (NaAlSi3O8) showing Si tetrahedra (blue), Al tetrahedra (green), Na atoms (yellow), and O atoms (red) visualized using VESTA.

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Works referenced in this record:

Rigidity Transition in Materials: Hardness is Driven by Weak Atomic Constraints
journal, March 2015

  • Bauchy, Mathieu; Qomi, Mohammad Javad Abdolhosseini; Bichara, Christophe
  • Physical Review Letters, Vol. 114, Issue 12
  • DOI: 10.1103/PhysRevLett.114.125502

Nature of radiation-induced defects in quartz
journal, July 2015

  • Wang, Bu; Yu, Yingtian; Pignatelli, Isabella
  • The Journal of Chemical Physics, Vol. 143, Issue 2
  • DOI: 10.1063/1.4926527

Modified model of alkali-silica reaction
journal, September 2007


Self-organization with equilibration: A model for the intermediate phase in rigidity percolation
journal, July 2006


Confined Water in Layered Silicates: The Origin of Anomalous Thermal Expansion Behavior in Calcium-Silicate-Hydrates
journal, December 2016

  • Krishnan, N. M. Anoop; Wang, Bu; Falzone, Gabriel
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 51
  • DOI: 10.1021/acsami.6b11587

Continuous deformations in random networks
journal, September 1983


Reactive Molecular Dynamics Simulations of Sodium Silicate Glasses - Toward an Improved Understanding of the Structure
journal, November 2016

  • Yu, Yingtian; Wang, Bu; Wang, Mengyi
  • International Journal of Applied Glass Science, Vol. 8, Issue 3
  • DOI: 10.1111/ijag.12248

Dielectric and infrared reflectance studies of inorganic oxide glasses
journal, June 1991


Albite dissolution kinetics as a function of distance from equilibrium: Implications for natural feldspar weathering
journal, March 2006


The effect of aluminum, pH, and chemical affinity on the rates of aluminosilicate dissolution reactions
journal, May 1994


Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995


Minerals from Macedonia. XXIV. Spectra-structure characterization of tectosilicates
journal, April 2009


VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011


Hard mode infrared spectroscopy of plagioclase feldspars [Hard mode infrared spectroscopy of plagioclase feldspars]
journal, February 1999

  • Atkinson, Alison J.; Carpenter, Michael A.; Salje, Ekhard K. H.
  • European Journal of Mineralogy, Vol. 11, Issue 1
  • DOI: 10.1127/ejm/11/1/0007

The pore solution of blended cements: a review
journal, October 2015

  • Vollpracht, Anya; Lothenbach, Barbara; Snellings, Ruben
  • Materials and Structures, Vol. 49, Issue 8
  • DOI: 10.1617/s11527-015-0724-1

Vertical Scanning Interferometry: A New Method to Measure the Dissolution Dynamics of Cementitious Minerals
journal, August 2013

  • Kumar, Aditya; Reed, Jason; Sant, Gaurav
  • Journal of the American Ceramic Society, Vol. 96, Issue 9
  • DOI: 10.1111/jace.12482

The albite structures
journal, August 1969

  • Ribbe, P. H.; Megaw, H. D.; Taylor, W. H.
  • Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 25, Issue 8
  • DOI: 10.1107/S0567740869004262

Steady-state kinetics and dissolution mechanisms of albite
journal, December 1985


Dispersion analysis of FTIR reflection measurements in silicate glasses
journal, September 2000

  • MacDonald, Steven A.; Schardt, Craig R.; Masiello, David J.
  • Journal of Non-Crystalline Solids, Vol. 275, Issue 1-2
  • DOI: 10.1016/S0022-3093(00)00121-6

Topology of covalent non-crystalline solids I: Short-range order in chalcogenide alloys
journal, October 1979


Dissolution kinetics as a function of the Gibbs free energy of reaction: An experimental study based on albite feldspar
journal, January 2006


The structure of high-silica alkali-silicate glasses. A Raman spectroscopic investigation
journal, November 1983

  • Matson, Dean W.; Sharma, Shiv K.; Philpotts, John A.
  • Journal of Non-Crystalline Solids, Vol. 58, Issue 2-3
  • DOI: 10.1016/0022-3093(83)90032-7

Structure and properties of sodium aluminosilicate glasses from molecular dynamics simulations
journal, July 2013

  • Xiang, Ye; Du, Jincheng; Smedskjaer, Morten M.
  • The Journal of Chemical Physics, Vol. 139, Issue 4
  • DOI: 10.1063/1.4816378

Swift heavy ion amorphization of quartz — a comparative study of the particle amorphization mechanism of quartz
journal, February 1996

  • Douillard, L.; Duraud, J. P.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 107, Issue 1-4
  • DOI: 10.1016/0168-583X(95)01044-0

Correlating the Network Topology of Oxide Glasses with their Chemical Durability
journal, January 2017

  • Mascaraque, Nerea; Bauchy, Mathieu; Smedskjaer, Morten M.
  • The Journal of Physical Chemistry B, Vol. 121, Issue 5
  • DOI: 10.1021/acs.jpcb.6b11371

Relation of expansion due to alkali silica reaction to the degree of reaction measured by SEM image analysis
journal, August 2007


Viscosity and viscosity anomalies of model silicates and magmas: A numerical investigation
journal, May 2013


Aragonite Undersaturation in the Arctic Ocean: Effects of Ocean Acidification and Sea Ice Melt
journal, November 2009


Molecular dynamics with coupling to an external bath
journal, October 1984

  • Berendsen, H. J. C.; Postma, J. P. M.; van Gunsteren, W. F.
  • The Journal of Chemical Physics, Vol. 81, Issue 8
  • DOI: 10.1063/1.448118

Order and disorder in calcium–silicate–hydrate
journal, June 2014

  • Bauchy, M.; Qomi, M. J. Abdolhosseini; Ulm, F. -J.
  • The Journal of Chemical Physics, Vol. 140, Issue 21
  • DOI: 10.1063/1.4878656

Molecular dynamics simulation of radiation damage in glasses
journal, July 2011


Constraint theory, vector percolation and glass formation
journal, February 1985


Effect of Nuclear Radiation on Alkali-Silica Reaction of Concrete
journal, October 2007


Role of surface speciation in the low-temperature dissolution of minerals
journal, February 1988

  • Blum, Alex; Lasaga, Antonio
  • Nature, Vol. 331, Issue 6155
  • DOI: 10.1038/331431a0

The infrared transmission spectra of four silicate glasses before and after exposure to water
journal, October 1990

  • Husung, Roy D.; Doremus, Robert H.
  • Journal of Materials Research, Vol. 5, Issue 10
  • DOI: 10.1557/JMR.1990.2209

An improved basis for characterizing the suitability of fly ash as a cement replacement agent
journal, June 2017

  • Oey, Tandré; Timmons, Jason; Stutzman, Paul
  • Journal of the American Ceramic Society, Vol. 100, Issue 10
  • DOI: 10.1111/jace.14974

Stretched Exponential Relaxation of Glasses at Low Temperature
journal, October 2015


Amorphization of SiC under ion and neutron irradiation
journal, May 1998

  • Snead, L. L.; Zinkle, S. J.; Hay, J. C.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 141, Issue 1-4
  • DOI: 10.1016/S0168-583X(98)00085-8

Crystal dissolution kinetics and Gibbs free energy
journal, February 2006


Direct Experimental Evidence for Differing Reactivity Alterations of Minerals following Irradiation: The Case of Calcite and Quartz
journal, January 2016

  • Pignatelli, Isabella; Kumar, Aditya; Field, Kevin G.
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep20155

L. On the calculation of the equilibrium and stiffness of frames
journal, April 1864

  • Maxwell, J. Clerk
  • The London, Edinburgh, and Dublin Philosophical Magazine and Journal of Science, Vol. 27, Issue 182
  • DOI: 10.1080/14786446408643668

An interferometric study of the dissolution kinetics of anorthite; the role of reactive surface area
journal, November 1999


Possibility of Radiation-Induced Degradation of Concrete by Alkali-Silica Reaction of Aggregates
journal, August 2002


On the use of SRIM for computing radiation damage exposure
journal, September 2013

  • Stoller, R. E.; Toloczko, M. B.; Was, G. S.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 310
  • DOI: 10.1016/j.nimb.2013.05.008

Gwyddion: an open-source software for SPM data analysis
journal, January 2012


The medium range structure of sodium silicate glasses: a molecular dynamics simulation
journal, December 2004


Effects of Al/Si ordering on feldspar dissolution: Part I. Crystallographic control on the stoichiometry of dissolution reaction
journal, February 2014


Dissolution of albite glass and crystal
journal, August 2000

  • Hamilton, James P.; Pantano, Carlo G.; Brantley, Susan L.
  • Geochimica et Cosmochimica Acta, Vol. 64, Issue 15
  • DOI: 10.1016/S0016-7037(00)00388-4

Topological Control on Silicates’ Dissolution Kinetics
journal, April 2016


Alkali–silica reaction: Current understanding of the reaction mechanisms and the knowledge gaps
journal, October 2015


Irradiation-induced topological transition in SiO2: Structural signature of networks' rigidity
journal, May 2017