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Understanding the Enhancement Mechanism of A-Site-Deficient LaxNiO3 as an Oxygen Redox Catalyst
Abstract
Lanthanide perovskite oxides have attracted much attention as an oxygen reduction and evolution catalyst because of their high chemical stability and composition adjustability. A defect strategy has been applied to enhance their electrocatalytic activity with the modulation of the crystal/electronic structure. However, the intrinsic roles of the defects, particularly A-site vacancies, are poorly understood. Herein, we prepare La x NiO 3 with various ratios of A-site vacancies by a facile nonstoichiometric strategy, which has boosted the dual-function catalytic activity of LaNiO 3 . More importantly, the enhancement mechanism of A-site-deficient La x NiO 3 as an oxygen redox catalyst has been unveiled. Induced vacancy defects on the A sites raise a compression strain in the NiO 6 octahedron, exerting a positive enhancement on Ni–O covalency. Furthermore, the e g electron filling in the active cation Ni and the overlapping state of Ni 3d–O 2p hybridization have also been optimized, in which renovation will further boost the catalytic ability of oxygen redox processes. This work not only clarifies the intrinsic roles of A-site deficiency in the structure and electrocatalytic activities of perovskite oxides but also presents some insights into the design and exploration of high-activity catalysts by cation defect modulation.
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“This defect saturation is the direct result of the La3+ deficiency, which generates a positive charge deficit that the system compensates for through vacancy formation and the reduction of metallic cations [47].”
From La-Co-Mn oxide aerogels as high-performance electrocatalysts for anion exchange membrane water electrolysis (2026) · cites this paper as [47]
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Metadata
- Authors
- Qiu, Y., Gao, R., Yang, W., Huang, L., Mao, Q., Yang, J., Sun, L., Hu, Z., & Liu, X.
- Affiliations
- University of Chinese Academy of Sciences (CN)
- China Institute of Atomic Energy (CN)
- Peking University (CN)
- Chinese Academy of Sciences (CN)
- Corresponding author
- Liu, Xiangfeng
- Venue
- Chemistry of Materials
- Publisher
- American Chemical Society (ACS)
- Published
- 2020-02-12
- Volume
- 32
- Issue
- 5
- Pages
- 1864-1875
- ISSN
- 0897-4756 (ISSN-L)
- 1520-5002
- OpenAlex
- W3006503774
- Cited by
- 105
- References
- 80
- Citations by year
- 2026: 21 · 2025: 19 · 2024: 18 · 2023: 16 · 2022: 13 · 2021: 14 · 2020: 4
- FWCI
- 2.32
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- Locations
- Chemistry of Materials (publishedVersion)
- Funders
- University of Chinese Academy of Sciences
- Natural Science Foundation of Beijing Municipality (2182082)
- National Natural Science Foundation of China (11575192, 11675267)
- Chinese Academy of Sciences (211211KYSB20170060, 211211KYSB20180020, XDB28000000, ZDKYYQ20170001)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › Advancements in Solid Oxide Fuel Cells
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Keywords
- LaNiO3, A-site vacancies, oxygen reduction reaction, oxygen evolution reaction, nonstoichiometry, defect engineering
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