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Main Authors: Ma, Hang, Liang, Ying, Ma, Tianxing, Linghu, Jiajun, Li, Zhi-Peng
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2503.07291
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author Ma, Hang
Liang, Ying
Ma, Tianxing
Linghu, Jiajun
Li, Zhi-Peng
author_facet Ma, Hang
Liang, Ying
Ma, Tianxing
Linghu, Jiajun
Li, Zhi-Peng
contents Proton-conducting solid oxide fuel cells (PC-SOFCs) are pivotal for their high proton conductivity and superior performance. The proton conduction mechanism is commonly described by the Grotthuss mechanism, involving proton rotation and transfer. While proton transfer is often considered the rate-limiting step, the underlying reasons remain unclear. Through density functional theory calculations on undoped, A-site doped, and B-site doped BaHfO$_3$ systems, we demonstrate that the rate-limiting nature of proton transfer stems from the formation of weaker hydrogen bonds. In systems with strong hydrogen bonds, proton rotation becomes non-negligible. We identify a critical hydrogen bond length that distinguishes strong from weak bonds, with shorter lengths correlating with distorted perovskite structures and configurations deviating from cubic. This insight into the necessity of rotation is crucial for screening and optimizing materials with superior proton conduction properties.
format Preprint
id arxiv_https___arxiv_org_abs_2503_07291
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Hydrogen Bond Strength Dictates the Rate-Limiting Steps of Diffusion in Proton-Conducting Perovskites:A Critical Length Perspective
Ma, Hang
Liang, Ying
Ma, Tianxing
Linghu, Jiajun
Li, Zhi-Peng
Materials Science
Proton-conducting solid oxide fuel cells (PC-SOFCs) are pivotal for their high proton conductivity and superior performance. The proton conduction mechanism is commonly described by the Grotthuss mechanism, involving proton rotation and transfer. While proton transfer is often considered the rate-limiting step, the underlying reasons remain unclear. Through density functional theory calculations on undoped, A-site doped, and B-site doped BaHfO$_3$ systems, we demonstrate that the rate-limiting nature of proton transfer stems from the formation of weaker hydrogen bonds. In systems with strong hydrogen bonds, proton rotation becomes non-negligible. We identify a critical hydrogen bond length that distinguishes strong from weak bonds, with shorter lengths correlating with distorted perovskite structures and configurations deviating from cubic. This insight into the necessity of rotation is crucial for screening and optimizing materials with superior proton conduction properties.
title Hydrogen Bond Strength Dictates the Rate-Limiting Steps of Diffusion in Proton-Conducting Perovskites:A Critical Length Perspective
topic Materials Science
url https://arxiv.org/abs/2503.07291