Amorphous SiO2 surface models: energetics of the dehydroxylation process, strain, ab initio atomistic thermodynamics and IR spectroscopic signatures

Physical Chemistry Chemical Physics : PCCP
Aleix Comas-Vives

Abstract

In this contribution, realistic amorphous SiO2 models of 2.1 × 2.1 nm with silanol densities ranging 1.1-7.2 OH per nm(2) are obtained by means of ab initio calculations via the dehydroxylation of a fully hydroxylated silica surface. The dehydroxyation process is considered to take place via direct condensation of adjacent silanol groups and silica migration steps. The latter reconstructions are needed in order to obtain highly dehydroxylated silica surfaces with favorable energetics and without the formation of defects. The obtained surface phase diagram of different silica models as a function of temperature and PH2O is able to correctly describe the silanol density under different conditions, and the IR spectroscopic signatures of the silanols are in qualitative agreement with the experiment. The amorphous silica models presented here have a high degree of heterogeneity as found from the big variability obtained in the energetics of the dehydroxylation steps. It was also found that the resulting average Si-O distance of the newly formed siloxane bridges serves as a descriptor of the strain introduced in the silica surface. All these factors can be crucial in order to simulate the activity of catalysts grafted onto silica wit...Continue Reading

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Citations

Jun 6, 2017·Journal of the American Chemical Society·Murielle F DelleyChristophe Copéret
Jun 14, 2017·Langmuir : the ACS Journal of Surfaces and Colloids·Daniel G GregoryMark A Snyder
Nov 26, 2016·Physical Chemistry Chemical Physics : PCCP·Maciej GieradaFrederik Tielens
May 29, 2018·Physical Chemistry Chemical Physics : PCCP·Ha-Linh Thi LeJean-Michel Mataigne
Dec 5, 2018·Nanotechnology·V V Afanas'evA Stesmans
Jun 25, 2019·Science and Technology of Advanced Materials·Bo Xiao, Satoshi Watanabe
May 16, 2020·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Valeri AfanasievVadim Trepalin
Jun 9, 2020·The Journal of Chemical Physics·Saber GueddidaSébastien Lebègue
Mar 23, 2017·Chemical Communications : Chem Comm·Aleix Comas-VivesChristophe Copéret
Sep 27, 2018·Physical Review. E·Zhuohan LiIzabela Szlufarska
Jan 1, 2021·The Journal of Chemical Physics·Craig A VanderveldenBaron Peters
Feb 19, 2021·Frontiers in Chemistry·Marco Fioroni, Nathan J DeYonker
Apr 6, 2021·Journal of the American Chemical Society·Maciej D KorzyńskiChristophe Copéret
Apr 17, 2021·Nature Materials·Thomas D BennettAndrew I Cooper
May 10, 2017·Chemistry of Materials : a Publication of the American Chemical Society·Adem YildirimAndrew P Goodwin
Feb 23, 2020·Journal of the American Chemical Society·Weizhong ZhengMichael D Fayer
Apr 13, 2020·Journal of Colloid and Interface Science·Y BerroA Pasc
Aug 7, 2017·Journal of Colloid and Interface Science·Anastasia SpyrogianniKarsten Wegner
Dec 29, 2021·Inorganic Chemistry·Frédéric A PerrasAaron D Sadow

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