Radiation-Induced Interfacial Hydroxyl Transformation on Boehmite and Gibbsite Basal Surfaces

Sassi, Michel; Walter, Eric D.; Qafoku, Odeta; Rosso, Kevin M.; Wang, Zheming

doi:10.1021/acs.jpcc.0c06844

Radiation-Induced Interfacial Hydroxyl Transformation on Boehmite and Gibbsite Basal Surfaces

Journal Article · Fri Sep 11 04:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c06844· OSTI ID:1721691

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)

Understanding the radiolytic reactivity of aluminum oxyhydroxide phases widely present in stored nuclear wastes is essential to develop reliable processing approaches. Recent experiments using vibrational sum frequency generation (VSFG), a surface sensitive technique, have shown that rehydration of γ-irradiated boehmite (010) and gibbsite (001) surfaces does not recover the initial hydroxyl density prior to irradiation. In this study, using density functional theory and nudged elastic band calculations, we examine dehydration and rehydration of these surfaces and attendant proton transfer mechanisms. While dehydration of both surfaces is predicted to be energetically unfavorable, rehydration of boehmite (010) is favorable after overcoming an energy barrier of 0.52 eV that relates to the orientation of surface hydroxyls controlling the hydrogen bonding network of adsorbed water. In the case of gibbsite (001), for which the experimental results suggest that rehydration mainly involves the reformation of interlayer hydroxyls, we found that a two-proton transfer mechanism is more likely than a one-proton transfer mechanism, and that it prevents the reorientation of interlayer hydroxyls into intralayer hydroxyls consistent with experimental VSFG findings. A detailed analysis of the effect of surface hydrogen vacancy on the strength of hydrogen bond interactions was performed, which indicates that H₂ and H₂O are the energetically most favorable product species to form from radiation-induced surface H and/or OH defects.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1721691

Report Number(s):: PNNL-SA-153541

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 40 Vol. 124; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (40)

Mesoporous Caged-γ-AlOOH-Double-Stranded RNA Analog Complexes for Cancer Immunotherapy Li, Xia; Shenashen, Mohamed A.; Wang, Xiupeng Advanced Biosystems, Vol. 2, Issue 1 https://doi.org/10.1002/adbi.201700114	journal	December 2017
Improved grid-based algorithm for Bader charge allocation Sanville, Edward; Kenny, Steven D.; Smith, Roger Journal of Computational Chemistry, Vol. 28, Issue 5 https://doi.org/10.1002/jcc.20575	journal	January 2007
Oxidation and Accumulation of H2 in the Aluminum-Water System Under the Radiation-Thermal Action Gadzhieva, N. N. Journal of Applied Spectroscopy, Vol. 72, Issue 4 https://doi.org/10.1007/s10812-005-0099-0	journal	July 2005
Radiolytic hydrogen generation from aluminum oxyhydroxide solids: theory and experiment Westbrook, M. L.; Sindelar, R. L.; Fisher, D. L. Journal of Radioanalytical and Nuclear Chemistry, Vol. 303, Issue 1 https://doi.org/10.1007/s10967-014-3563-6	journal	November 2014
A fast and robust algorithm for Bader decomposition of charge density Henkelman, Graeme; Arnaldsson, Andri; Jónsson, Hannes Computational Materials Science, Vol. 36, Issue 3 https://doi.org/10.1016/j.commatsci.2005.04.010	journal	June 2006
High-strength boehmite-acrylate composites for 3D printing: Reinforced filler-matrix interactions Han, Yanyang; Wang, FuKe; Wang, Haimei Composites Science and Technology, Vol. 154 https://doi.org/10.1016/j.compscitech.2017.10.026	journal	January 2018
Characterization of O–H⋯O interactions in linear and cyclic clusters of boric acid: An ab initio, DFT, QTAIM and NBO study Esrafili, Mehdi D.; Alizadeh, Vahideh Computational and Theoretical Chemistry, Vol. 974, Issue 1-3 https://doi.org/10.1016/j.comptc.2011.07.019	journal	November 2011
Critic: a new program for the topological analysis of solid-state electron densities Otero-de-la-Roza, A.; Blanco, M. A.; Pendás, A. Martín Computer Physics Communications, Vol. 180, Issue 1 https://doi.org/10.1016/j.cpc.2008.07.018	journal	January 2009
Variable cell nudged elastic band method for studying solid–solid structural phase transitions Qian, Guang-Rui; Dong, Xiao; Zhou, Xiang-Feng Computer Physics Communications, Vol. 184, Issue 9 https://doi.org/10.1016/j.cpc.2013.04.004	journal	September 2013
Critic2: A program for real-space analysis of quantum chemical interactions in solids Otero-de-la-Roza, A.; Johnson, Erin R.; Luaña, Víctor Computer Physics Communications, Vol. 185, Issue 3 https://doi.org/10.1016/j.cpc.2013.10.026	journal	March 2014
Efficient hydrogen production from irradiated aluminum hydroxides Kaddissy, Josiane A.; Esnouf, Stéphane; Saffré, Dimitri International Journal of Hydrogen Energy, Vol. 44, Issue 7 https://doi.org/10.1016/j.ijhydene.2018.12.089	journal	February 2019
The role of surface hydroxyls on the radiolysis of gibbsite and boehmite nanoplatelets Wang, Zheming; Walter, Eric D.; Sassi, Michel Journal of Hazardous Materials, Vol. 398 https://doi.org/10.1016/j.jhazmat.2020.122853	journal	November 2020
Radiolytic stability of gibbsite and boehmite with adsorbed water Huestis, Patricia; Pearce, Carolyn I.; Zhang, X. Journal of Nuclear Materials, Vol. 501 https://doi.org/10.1016/j.jnucmat.2018.01.043	journal	April 2018
Alumina Hydrate Polymorphism Control in Al–Water Reaction Crystallization by Seeding to Change the Metastable Zone Width Wang, Hongqi; Wang, Zhi; Liu, Ling Crystal Growth & Design, Vol. 16, Issue 2 https://doi.org/10.1021/acs.cgd.5b01620	journal	January 2016
Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site Peterson, Reid A.; Buck, Edgar C.; Chun, Jaehun Environmental Science & Technology, Vol. 52, Issue 2 https://doi.org/10.1021/acs.est.7b04077	journal	January 2018
Evolution of Radicals from the Photolysis of High Ionic Strength Alkaline Nitrite Solutions Walter, Eric D.; Schwarz, Kaitlynn C.; Kumar, Shweta Anil The Journal of Physical Chemistry A, Vol. 124, Issue 16 https://doi.org/10.1021/acs.jpca.9b11438	journal	March 2020
Surface Hydration and Hydroxyl Configurations of Gibbsite and Boehmite Nanoplates Sassi, Michel; Wang, Zheming; Walter, Eric D. The Journal of Physical Chemistry C, Vol. 124, Issue 9 https://doi.org/10.1021/acs.jpcc.0c00659	journal	February 2020
Radiolytic Events in Nanostructured Aluminum Hydroxides Kaddissy, Josiane A.; Esnouf, Stephane; Durand, Delphine The Journal of Physical Chemistry C, Vol. 121, Issue 11 https://doi.org/10.1021/acs.jpcc.6b13104	journal	March 2017
Molecular Dynamics Simulations of the Interfacial Region between Boehmite and Gibbsite Basal Surfaces and High Ionic Strength Aqueous Solutions Shen, Zhizhang; Ilton, Eugene S.; Prange, Micah P. The Journal of Physical Chemistry C, Vol. 121, Issue 25 https://doi.org/10.1021/acs.jpcc.7b02463	journal	June 2017
Diffusion Mechanisms of Radiolytic Species in Irradiated Al (Oxy-)Hydroxides Shen, Zhizhang; Ilton, Eugene S.; Prange, Micah P. The Journal of Physical Chemistry C, Vol. 122, Issue 50 https://doi.org/10.1021/acs.jpcc.8b07809	journal	November 2018
Separation of Radiolytic Species at the Boehmite–Water Interface Kerisit, Sebastien N.; Shen, Zhizhang; Prange, Micah P. The Journal of Physical Chemistry C, Vol. 123, Issue 25 https://doi.org/10.1021/acs.jpcc.9b02144	journal	May 2019
Electron- and Thermal-Stimulated Synthesis of Water on Boehmite (γ-AlOOH) Nanoplates Jones, Brant M.; Aleksandrov, Alexandr; Zhang, Xin The Journal of Physical Chemistry C, Vol. 123, Issue 31 https://doi.org/10.1021/acs.jpcc.9b03927	journal	July 2019
Theoretical Study of Dihydrogen Bonds between (XH) ₂ , X = Li, Na, BeH, and MgH, and Weak Hydrogen Bond Donors (HCN, HNC, and HCCH) Alkorta, Ibon; Zborowski, Krzysztof; Elguero, Jose The Journal of Physical Chemistry A, Vol. 110, Issue 34 https://doi.org/10.1021/jp061481x	journal	August 2006
The Perdew–Burke–Ernzerhof exchange-correlation functional applied to the G2-1 test set using a plane-wave basis set Paier, Joachim; Hirschl, Robin; Marsman, Martijn The Journal of Chemical Physics, Vol. 122, Issue 23 https://doi.org/10.1063/1.1926272	journal	June 2005
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu Grimme, Stefan; Antony, Jens; Ehrlich, Stephan The Journal of Chemical Physics, Vol. 132, Issue 15 https://doi.org/10.1063/1.3382344	journal	April 2010
Accurate and efficient algorithm for Bader charge integration Yu, Min; Trinkle, Dallas R. The Journal of Chemical Physics, Vol. 134, Issue 6 https://doi.org/10.1063/1.3553716	journal	February 2011
Cooperative (nonpairwise) effects in water trimers: An ab initio molecular orbital study Mó, O.; Yáñez, M.; Elguero, J. The Journal of Chemical Physics, Vol. 97, Issue 9 https://doi.org/10.1063/1.463666	journal	November 1992
Electronic response of aluminum-bearing minerals Prange, Micah P.; Zhang, Xin; Ilton, Eugene S. The Journal of Chemical Physics, Vol. 149, Issue 2 https://doi.org/10.1063/1.5037104	journal	July 2018
A grid-based Bader analysis algorithm without lattice bias Tang, W.; Sanville, E.; Henkelman, G. Journal of Physics: Condensed Matter, Vol. 21, Issue 8 https://doi.org/10.1088/0953-8984/21/8/084204	journal	January 2009
An ab initio study on the transition paths from graphite to diamond under pressure Dong, Xiao; Zhou, Xiang-Feng; Qian, Guang-Rui Journal of Physics: Condensed Matter, Vol. 25, Issue 14 https://doi.org/10.1088/0953-8984/25/14/145402	journal	March 2013
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)] Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 78, Issue 7 https://doi.org/10.1103/PhysRevLett.78.1396	journal	February 1997
Comment on “Generalized Gradient Approximation Made Simple” Zhang, Yingkai; Yang, Weitao Physical Review Letters, Vol. 80, Issue 4 https://doi.org/10.1103/PhysRevLett.80.890	journal	January 1998
Hydrogen Atoms in Boehmite: A Single Crystal X-Ray Diffraction and Molecular Orbital Study Hill, Roderick J. Clays and Clay Minerals, Vol. 29, Issue 6 https://doi.org/10.1346/CCMN.1981.0290604	journal	January 1981
Refinement of the crystal structure of gibbsite, Al(OH) ₃ Saalfeld, H.; Wedde, M. Zeitschrift für Kristallographie, Vol. 139, Issue 1-2 https://doi.org/10.1524/zkri.1974.139.1-2.129	journal	April 1974
Assignment of the structural OH stretching bands of gibbsite Wang, Shan-Li; Johnston, Cliff T. American Mineralogist, Vol. 85, Issue 5-6 https://doi.org/10.2138/am-2000-5-612	journal	May 2000
Gold nanocages for cancer detection and treatment Skrabalak, Sara E.; Au, Leslie; Lu, Xianmao Nanomedicine, Vol. 2, Issue 5 https://doi.org/10.2217/17435889.2.5.657	journal	October 2007

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