First-Principles Insight into the Effects of Intrinsic Oxygen Defects on Proton Conduction in Ruddlesden–Popper Oxides
First-Principles Insight into the Effects of Intrinsic Oxygen Defects on Proton Conduction in Ruddlesden–Popper Oxides
复制标题
第一性原理洞察本征氧缺陷对 Ruddlesden-Popper 氧化物中质子传导的影响
DOI：
10.1021/acs.jpclett.1c02749
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发表时间：
2021
影响因子：
5.7
通讯作者：
Linjuan Zhang
中科院分区：
文献类型：
--
作者：
Lili Li;Jing Zhou;Zhiwei Hu;Sihyuk Choi;Guntae Kim;Jianqiang Wang;Linjuan Zhang
了解质子输运Ruddlesden-Popper（RP）氧化物，作为有吸引力的电极材料的质子陶瓷燃料电池，是具有挑战性的，因为在第一系列RP氧化物（A2 BO 4）的固有氧缺陷的复杂性。我们研究了A2 BO 4中本征氧缺陷在质子输运中的过程，如缺陷的形成、游离水的掺入、质子沿着氧位的转移以及过渡态的电子性质.氧空位（VO）和间隙氧（Oi）的共存（VO+Oi缺陷对）呈现有利的水合能和晶格畸变，有效地加速了晶格中的质子输运。此外，TS中的O-H···O键相互作用使质子输运的内在驱动力与O 2 p带能级有关.我们的研究结果阐明了质子传导受内在氧缺陷影响的基本机制，这将促使社会更加关注缺陷工程，以提高性能。
Understanding proton transport in Ruddlesden-Popper (RP) oxides, as attractive electrode materials for protonic ceramic fuel cells, is challenging because of the complexity of intrinsic oxygen defects in first-series RP oxides (A2BO4). We investigated the processes of intrinsic oxygen defects in proton transportation, such as formation of defects, incorporation of dissociative water into the defective lattice, transfer of a proton along the oxygen sites, and electronic properties of the transition state (TS) in A2BO4. The coexistence of oxygen vacancies (VO) and interstitial oxygen (Oi), VO+Oi defect pair, presents advantageous hydration energies and lattice distortions efficiently accelerating proton transport in the lattice. Moreover, the inherent driving force for proton transport is related to the O 2p band level by O-H···O bond interactions in the TS. Our findings elucidate the fundamental mechanism of proton conduction affected by intrinsic oxygen defects, which will motivate the community to focus more on defect engineering to enhance performance.