Dynamics of self-reorganization explains passivation of silicate glasses

被引:112
作者
Gin, Stephane [1 ]
Collin, Marie [1 ]
Jollivet, Patrick [1 ]
Fournier, Maxime [1 ]
Minet, Yves [1 ]
Dupuy, Laurent [2 ]
Mahadevan, Thiruvilla [3 ]
Kerisit, Sebastien [4 ]
Du, Jincheng [3 ]
机构
[1] CEA, DEN, DE2D, SEVT, F-30207 Bagnols Sur Ceze, France
[2] ZAC St Charles, Tescan Analyt, F-13710 Fuveau, France
[3] Univ North Texas, Dept Mat Sci & Engn, Denton, TX 76203 USA
[4] Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99352 USA
关键词
NUCLEAR-WASTE GLASS; DIFFUSION COEFFICIENTS; WATER; CORROSION; SIMULATIONS; MECHANISMS; MINERALS; POROSITY; SIZE;
D O I
10.1038/s41467-018-04511-2
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Understanding the dissolution of silicate glasses and minerals from atomic to macroscopic levels is a challenge with major implications in geoscience and industry. One of the main uncertainties limiting the development of predictive models lies in the formation of an amorphous surface layer--called gel--that can in some circumstances control the reactivity of the buried interface. Here, we report experimental and simulation results deciphering the mechanisms by which the gel becomes passivating. The study conducted on a six-oxide borosilicate glass shows that gel reorganization involving high exchange rate of oxygen and low exchange rate of silicon is the key mechanism accounting for extremely low apparent water diffusivity (similar to 10(-21) m(2) s(-1)), which could be rate-limiting for the overall reaction. These findings could be used to improve kinetic models, and inspire the development of new molecular sieve materials with tailored properties as well as highly durable glass for application in extreme environments.
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页数:9
相关论文
共 37 条
[1]   Molecular Dynamics Simulations of Water Structure and Diffusion in Silica Nanopores [J].
Bourg, Ian C. ;
Steefel, Carl I. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2012, 116 (21) :11556-11564
[2]   Why Do Certain Glasses with a High Dissolution Rate Undergo a Low Degree of Corrosion? [J].
Cailleteau, Celine ;
Devreux, Francois ;
Spalla, Olivier ;
Angeli, Frederic ;
Gin, Stephane .
JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (13) :5846-5855
[3]   Insight into silicate-glass corrosion mechanisms [J].
Cailleteau, Celine ;
Angeli, Frederic ;
Devreux, Francois ;
Gin, Stephane ;
Jestin, Jacques ;
Jollivet, Patrick ;
Spalla, Olivier .
NATURE MATERIALS, 2008, 7 (12) :978-983
[4]   LEACHING AND RECONSTRUCTION AT THE SURFACES OF DISSOLVING CHAIN-SILICATE MINERALS [J].
CASEY, WH ;
WESTRICH, HR ;
BANFIELD, JF ;
FERRUZZI, G ;
ARNOLD, GW .
NATURE, 1993, 366 (6452) :253-256
[5]  
Collin M., 2018, NPJ MAT DEGRAD, V2
[6]   Impact of alkali on the passivation of silicate glass [J].
Collin, Marie ;
Fournier, Maxime ;
Charpentier, Thibault ;
Moskura, Melanie ;
Gin, Stephane .
NPJ MATERIALS DEGRADATION, 2018, 2 (01)
[7]   Dynamics of altered surface layer formation on dissolving silicates [J].
Daval, Damien ;
Bernard, Sylvain ;
Remusat, Laurent ;
Wild, Bastien ;
Guyot, Francois ;
Micha, Jean Sebastien ;
Rieutord, Francois ;
Magnin, Valerie ;
Fernandez-Martinez, Alejandro .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2017, 209 :51-69
[8]   DIFFUSION OF WATER IN SILICA GLASS [J].
DOREMUS, RH .
JOURNAL OF MATERIALS RESEARCH, 1995, 10 (09) :2379-2389
[9]   Water diffusion in the simulated French nuclear waste glass SON 68 contacting silica rich solutions: Experimental and modeling [J].
Ferrand, K. ;
Abdelouas, A. ;
Grambow, B. .
JOURNAL OF NUCLEAR MATERIALS, 2006, 355 (1-3) :54-67
[10]   SON68 nuclear glass dissolution kinetics: Current state of knowledge and basis of the new GRAAL model [J].
Frugier, P. ;
Gin, S. ;
Minet, Y. ;
Chave, T. ;
Bonin, B. ;
Godon, N. ;
Lartigue, J. -E. ;
Jollivet, P. ;
Ayral, A. ;
De Windt, L. ;
Santarini, G. .
JOURNAL OF NUCLEAR MATERIALS, 2008, 380 (1-3) :8-21