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Vol. 16 (2024)

Accelerating Oxygen Electrocatalysis Kinetics on Metal–Organic Frameworks via Bond Length Optimization

https://doi.org/10.1007/s40820-024-01382-9
Fan He
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Yingnan Liu
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Xiaoxuan Yang
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Yaqi Chen
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Cheng‑Chieh Yang
Department of Physics, Tamkang University, New Taipei 25137, Taiwan, People’s Republic of China
Chung‑Li Dong
Department of Physics, Tamkang University, New Taipei 25137, Taiwan, People’s Republic of China
Qinggang He
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Bin Yang
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Zhongjian Li
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Yongbo Kuang
Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, People’s Republic of China
Lecheng Lei
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Liming Dai
Australian Carbon Materials Centre (A‑CMC), School of Chemical Engineering, University of New South Wales, Sydney, NSW 2051, Australia
Yang Hou
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China

Corresponding Author: Yang Hou

yhou@zju.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 175

Abstract

Metal–organic frameworks (MOFs) have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity, but the limited catalytic activity and stability has hampered their practical use in water splitting. Herein, we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs (donated as AE-CoNDA) to serve as efficient catalyst for water splitting. AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm−2 and a small Tafel slope of 62 mV dec−1 with excellent stability over 100 h. After integrated AE-CoNDA onto BiVO4, photocurrent density of 4.3 mA cm−2 is achieved at 1.23 V. Experimental investigations demonstrate that the stretched Co–O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p, which accounts for the fast kinetics and high activity. Theoretical calculations reveal that the stretched Co–O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.


Highlights:
1 The acid etching Co-naphthalenedicarboxylic acid-based metal–organic frameworks (donated as AE-CoNDA) catalyst displayed an excellent oxygen evolution reaction (OER) activity for long-term stability.
2 Integration of the AE-CoNDA cocatalyst into BiVO4 achieved a remarkable PEC-OER activity.
3 The stretched Co-O bond length regulated the spin state transition at the Co active sites.
4 The optimized high spin state of Co sites adjusted the orbitals hybridization of Co 3d and O 2p.

Keywords

Metal–organic frameworks Bond length adjustment Spin state transition Orbitals hybridization Water splitting
He, Fan, Yingnan Liu, Xiaoxuan Yang, Yaqi Chen, Cheng‑Chieh Yang, Chung‑Li Dong, Qinggang He, Bin Yang, Zhongjian Li, Yongbo Kuang, Lecheng Lei, Liming Dai, and Yang Hou. 2024. “Accelerating Oxygen Electrocatalysis Kinetics on Metal–Organic Frameworks via Bond Length Optimization”. Nano-Micro Letters 16 (April):175. https://doi.org/10.1007/s40820-024-01382-9.
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