Defect Chemistry and Hydrogen Transport in La/Sr-Based Oxyhydrides

Rowberg, Andrew J. E.; Weston, Leigh; Van de Walle, Chris G.

doi:10.1021/acs.jpcc.0c09222

Title: Defect Chemistry and Hydrogen Transport in La/Sr-Based Oxyhydrides

Journal Article · Tue Jan 26 00:00:00 EST 2021 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c09222· OSTI ID:1762494

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Univ. of California, Santa Barbara, CA (United States)
Univ. of California, Santa Barbara, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Oxyhydrides in the series La_{2 – y}Sr_yLiH_{1 + y}O_{3 – y} are attractive materials for solid-state hydride electrolytes. However, their chemical stability is poor, and thus far only La₂LiHO₃ (y = 0) has been demonstrated in a working fuel cell. Using a first-principles approach to study defect chemistry and stability, we find that La₂LiHO₃ can be stabilized over a range of H-rich, O-poor chemical conditions, while Sr₂LiH₃O has low stability. Here, defects are critical for ionic transport and for stability, particularly in Sr₂LiH₃O, in which anion antisites and H vacancies readily form. In fact, we show that the ground-state structure of Sr₂LiH₃O is inherently disordered. La₂LiHO₃ has low conductivity, which we connect to the high formation energy of defects such as VO and OH that are necessary for hydride conduction. When Sr₂LiH₃O is grown under carefully selected conditions, V_H⁺ defects can be made prevalent; these defects give rise to much higher ionic conductivity than can be obtained in La₂LiHO₃. In general, we show that the choice of synthesis conditions is vital when seeking to optimize the stability and ionic conductivity of these oxyhydrides, thereby tailoring them for use in solid-state hydrogen fuel cells.

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Research Organization:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Contributing Organization:: Center for Scientific Computing, supported by the California NanoSystems Institute and the Materials Research Science and Engineering Center (NSF); National Energy Research Scientific Computing Center (DOE, DE-AC02-05CH11231)

Grant/Contract Number:: FG02-07ER46434; AC02-05CH11231

OSTI ID:: 1762494

Journal Information:: Journal of Physical Chemistry. C, Vol. 125, Issue 4; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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