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- Title
Unusual double ligand holes as catalytic active sites in LiNiO<sub>2</sub>.
- Authors
Huang, Haoliang; Chang, Yu-Chung; Huang, Yu-Cheng; Li, Lili; Komarek, Alexander C.; Tjeng, Liu Hao; Orikasa, Yuki; Pao, Chih-Wen; Chan, Ting-Shan; Chen, Jin-Ming; Haw, Shu-Chih; Zhou, Jing; Wang, Yifeng; Lin, Hong-Ji; Chen, Chien-Te; Dong, Chung-Li; Kuo, Chang-Yang; Wang, Jian-Qiang; Hu, Zhiwei; Zhang, Linjuan
- Abstract
Designing efficient catalyst for the oxygen evolution reaction (OER) is of importance for energy conversion devices. The anionic redox allows formation of O-O bonds and offers higher OER activity than the conventional metal sites. Here, we successfully prepare LiNiO2 with a dominant 3d8L configuration (L is a hole at O 2p) under high oxygen pressure, and achieve a double ligand holes 3d8L2 under OER since one electron removal occurs at O 2p orbitals for NiIII oxides. LiNiO2 exhibits super-efficient OER activity among LiMO2, RMO3 (M = transition metal, R = rare earth) and other unary 3d catalysts. Multiple in situ/operando spectroscopies reveal NiIII→NiIV transition together with Li-removal during OER. Our theory indicates that NiIV (3d8L2) leads to direct O-O coupling between lattice oxygen and *O intermediates accelerating the OER activity. These findings highlight a new way to design the lattice oxygen redox with enough ligand holes created in OER process. Lattice-oxygen redox is pivotal for high oxygen evolution reaction (OER) activity. Here, LiNiO2, a unary 3d-transition metal oxide catalyst, exhibits superefficient activity during the OER due to the creation of double O 2p holes states, according to operando XAS, XRD, and Raman spectroscopy observations.
- Subjects
OXYGEN evolution reactions; TRANSITION metal oxides; RARE earth oxides; METALLIC oxides; METAL catalysts; TRANSITION metals
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-37775-4