First principles simulations of MgO(100) surface hydration at ambient conditions

Sassi, Michel; Rosso, Kevin M.

doi:10.1039/d3cp04848a

Title: First principles simulations of MgO(100) surface hydration at ambient conditions

Journal Article · 18 December 2023 · Physical Chemistry Chemical Physics. PCCP

DOI: https://doi.org/10.1039/d3cp04848a · OSTI ID:2274864

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

Developing a better understanding of water ordering and hydroxylation at oxide mineral surfaces is important across a breath of application spaces. Recent vibrational sum frequency generation (vSFG) measurements on MgO(100) surfaces at ambient conditions showed that water dissociates and hydroxylates the surface yielding a non-hydrogen bonded hydroxyl species. Starting from previously determined water hydroxylation patterns on MgO(100), we performed ab initio thermodynamic calculations and vibrational analysis to compare with the vSFG observations. At ambient conditions (i.e., T = 298.15 K and pH₂O = 32 mbar), the most thermodynamically favorable surface hydroxylation is found to be p(3 × 2) – 8H₂O, involving a dissociation of 25% of the adsorbed water. Analysis of the vibrational density of states for this hydroxylation configuration yielded three different hydrogen bonding environments with the frequency of the peaks in very good agreement with the vSFG measurements. However, the non-H-bonded spectral feature on this surface is predicted to be similar to that expected for Mg(OH)₂, a thermodynamically downhill alteration of the surface that must be independently ruled out before one can be fully confident in the apparent theory/vSFG agreement. Our study provides more insights into the ordering and structure of water monolayer at MgO(100) surface at ambient conditions and completes previous theoretical and experimental analysis performed at low temperature and ultra-high vacuum conditions.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE

Grant/Contract Number:: AC05-76RL01830; FWP 56674

OSTI ID:: 2274864

Alternate ID(s):: OSTI ID: 2348878

Report Number(s):: PNNL-SA-188183

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Vol. 26, Issue 3; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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