Elucidating the temperature and density dependence of silver chloride hydration numbers in high-temperature water vapor: A first-principles molecular simulation study

Messerly, Richard Alma; Yoon, Tae-Jun; Jadrich, Ryan Bradley; Currier, Robert Patrick; Maerzke, Katie A.

doi:10.1016/j.chemgeo.2022.120766

Title: Elucidating the temperature and density dependence of silver chloride hydration numbers in high-temperature water vapor: A first-principles molecular simulation study

Journal Article · 10 February 2022 · Chemical Geology

DOI: https://doi.org/10.1016/j.chemgeo.2022.120766 · OSTI ID:1846147

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Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Hydration numbers of metal complexes in low-density aqueous solutions are required for developing geochemical models for ore-forming metals and for designing supercritical desalination processes. In this study, we investigate the temperature and density dependence of the hydration numbers of silver chloride at 623 K, 673 K, and 713 K and densities of 10–100 kg/m³. Experimental estimates of the hydration number in the literature for AgCl at these conditions are inconclusive and possibly contradictory as to the temperature and density dependence. First-principles molecular simulation presents an attractive alternative to experimental measurements. Specifically, recent work shows that machine-learning-accelerated nested Monte Carlo simulations provide reliable estimates for the hydration numbers of CuCl at 623 K from 10 to 100 kg/m³. Using the same technique, we find a monotonic temperature dependence, with the hydration number decreasing slightly with increasing temperature. In addition, the simulation-predicted hydration numbers steadily increase with increasing density. These temperature and density trends are in agreement with certain experimental data sets. Therefore, this work demonstrates how first-principles Monte Carlo simulations assist in resolving discrepancies between experimental data sets. Our simulation results also correctly predict that the hydration number, and thus also the solubility, of AgCl is lower than that of CuCl under the same conditions. Furthermore, the bond length and angle formed between the water complex and AgCl differ from those for CuCl, consistent with the lower solubility of AgCl.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1846147

Report Number(s):: LA-UR--21-29838

Journal Information:: Chemical Geology, Journal Name: Chemical Geology Vol. 594; ISSN 0009-2541

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Elucidating the temperature and density dependence of silver chloride hydration numbers in high-temperature water vapor: A first-principles molecular simulation study

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