A Computational Framework to Accelerate the Discovery of Perovskites for Solar Thermochemical Hydrogen Production: Identification of Gd Perovskite Oxide Redox Mediators

Bare, Zachary L.; Morelock, Ryan J.; Musgrave, Charles B.

doi:10.1002/adfm.202200201

Title: A Computational Framework to Accelerate the Discovery of Perovskites for Solar Thermochemical Hydrogen Production: Identification of Gd Perovskite Oxide Redox Mediators

Journal Article · Sun Mar 20 00:00:00 EDT 2022 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202200201· OSTI ID:1976187

Bare, Zachary L. ^[1]; Morelock, Ryan J. ^[1];

^[1]

University of Colorado, Boulder, CO (United States)

Abstract A high‐throughput computational framework to identify novel multinary perovskite redox mediators is presented, and this framework is applied to discover the Gd‐containing perovskite oxide compositions Gd ₂ BB′O _6, GdA′B ₂ O ₆ , and GdA′BB′O ₆ that split water. The computational scheme uses a sequence of empirical approaches to evaluate the stabilities, electronic properties, and oxygen vacancy thermodynamics of these materials, including contributions to the enthalpies and entropies of reduction, Δ H _TR and Δ S _TR . This scheme uses the machine‐learned descriptor τ to identify compositions that are likely stable as perovskites, the bond valence method to estimate the magnitude and phase of BO ₆ octahedral tilting and provide accurate initial estimates of perovskite geometries, and density functional theory including magnetic‐ and defect‐sampling to predict STCH‐relevant properties. Eighty‐three promising STCH candidate perovskite oxides down‐selected from 4392 Gd‐containing compositions are reported, three of which are referred to experimental collaborators for characterization and exhibit STCH activity. The results demonstrate that the high‐throughput computational scheme described herein—which is used to evaluate Gd‐containing compositions but can be applied to any multinary perovskite oxide compositional space(s) of interest—accelerates the discovery of novel STCH active redox mediators with reasonable computational expense.

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Research Organization:: Univ. of Colorado, Boulder, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); National Science Foundation (NSF); University of Colorado; USDOE

Grant/Contract Number:: EE0008088; CHEM-1800592; CBET-2016225; P200A180012

OSTI ID:: 1976187

Alternate ID(s):: OSTI ID: 1856536

Journal Information:: Advanced Functional Materials, Vol. 32, Issue 25; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: A Computational Framework to Accelerate the Discovery of Perovskites for Solar Thermochemical Hydrogen Production: Identification of Gd Perovskite Oxide Redox Mediators

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