Ligand vacancy channels in pillared inorganic-organic hybrids for electrocatalytic organic oxidation with enzyme-like activities

Zhe Chen, Jili Li, Lingshen Meng, Jianan Li, Yaming Hao, Tao Jiang, Xuejing Yang, Yefei Li (), Zhi-Pan Liu and Ming Gong ()
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Zhe Chen: Fudan University
Jili Li: Fudan University
Lingshen Meng: Fudan University
Jianan Li: East China University of Science and Technology
Yaming Hao: Fudan University
Tao Jiang: Fudan University
Xuejing Yang: East China University of Science and Technology
Yefei Li: Fudan University
Zhi-Pan Liu: Fudan University
Ming Gong: Fudan University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Simultaneously achieving abundant and well-defined active sites with high selectivity has been one of the ultimate goals for heterogeneous catalysis. Herein, we construct a class of Ni hydroxychloride-based inorganic-organic hybrid electrocatalysts with the inorganic Ni hydroxychloride chains pillared by the bidentate N-N ligands. The precise evacuation of N-N ligands under ultrahigh-vacuum forms ligand vacancies while partially retaining some ligands as structural pillars. The high density of ligand vacancies forms the active vacancy channel with abundant and highly-accessible undercoordinated Ni sites, exhibiting 5-25 fold and 20-400 fold activity enhancement compared to the hybrid pre-catalyst and standard β-Ni(OH)2 for the electrochemical oxidation of 25 different organic substrates, respectively. The tunable N-N ligand can also tailor the sizes of the vacancy channels to significantly impact the substrate configuration leading to unprecedented substrate-dependent reactivities on hydroxide/oxide catalysts. This approach bridges heterogenous and homogeneous catalysis for creating efficient and functional catalysis with enzyme-like properties.

Date: 2023
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DOI: 10.1038/s41467-023-36830-4

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