Highly Active Surface Structure in Nanosized Spinel Cobalt-Based Oxides for Electrocatalytic Water Splitting | |
Zhou, J; Li, J; Zhang, LJ; Song, SZ; Wang, Y; Lin, X; Gu, SQ; Wu, X; Weng, TC; Wang, JQ | |
刊名 | JOURNAL OF PHYSICAL CHEMISTRY C
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2018 | |
卷号 | 122期号:26页码:14447-14458 |
关键词 | OXYGEN-EVOLVING CATALYSTS X-RAY-ABSORPTION OCTAHEDRAL SYMMETRY STATE TRANSITION NANOWIRE ARRAYS CRYSTAL PLANE FUEL-CELLS EVOLUTION OXIDATION PEROVSKITE |
ISSN号 | 1932-7447 |
DOI | 10.1021/acs.jpcc.8b00407 |
文献子类 | 期刊论文 |
英文摘要 | Spinel cobalt-based oxides are a promising family of materials for water splitting to replace currently used noble-metal catalysts. Identifying the highly active facet and the corresponding coordinated structure of surface redox centers is pivotal for the rational design of low-cost and efficient nanosized catalysts. Using high-resolution transmission electron microscopy and advanced X-ray techniques, as well as ab initio modeling, we found that the activity of Co3+ ions exhibits the surface dependence owing to the variability of its electronic configurations. Our calculation shows that the Co3+ site in {100} facet of nanosized Li2Co2O4 exhibits an impressive intrinsic activity with low overpotential, far lower than that of the {110} and {111} facets. The unique, well-defined CoO5 square-pyramidal structure in this nonpolar surface stabilizes the unusual intermediate-spin states of the Co3+ ion. Specially, we unraveled that oxygen ion anticipates the redox process via the strong hybridization Co 3d-O 2p state, which produces a 3d(z)(21.1) filling orbit. Finally, a spin-correlated energy diagram as a function of Co-O distance was devised, showing that the covalency of Co-O significantly affects the spin state of Co3+ ions. We suggest that the nonpolar surface that contains CoO5 units in the edge-sharing systems with the short Co-O bond distance is a potential candidate for alkaline water electrolysis. |
语种 | 英语 |
内容类型 | 期刊论文 |
源URL | [http://ir.sinap.ac.cn/handle/331007/30969] ![]() |
专题 | 上海应用物理研究所_中科院上海应用物理研究所2011-2017年 |
作者单位 | 1.China Univ Geosci, State Key Lab Geol Proc & Mineral Resources, Wuhan 430074, Hubei, Peoples R China 2.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201204, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.Ctr High Pressure Sci & Technol Adv Res, Shanghai 201203, Peoples R China |
推荐引用方式 GB/T 7714 | Zhou, J,Li, J,Zhang, LJ,et al. Highly Active Surface Structure in Nanosized Spinel Cobalt-Based Oxides for Electrocatalytic Water Splitting[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2018,122(26):14447-14458. |
APA | Zhou, J.,Li, J.,Zhang, LJ.,Song, SZ.,Wang, Y.,...&Zhang, S.(2018).Highly Active Surface Structure in Nanosized Spinel Cobalt-Based Oxides for Electrocatalytic Water Splitting.JOURNAL OF PHYSICAL CHEMISTRY C,122(26),14447-14458. |
MLA | Zhou, J,et al."Highly Active Surface Structure in Nanosized Spinel Cobalt-Based Oxides for Electrocatalytic Water Splitting".JOURNAL OF PHYSICAL CHEMISTRY C 122.26(2018):14447-14458. |
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