Oxygen‐coordinated low‐nucleus cluster catalysts for enhanced electrocatalytic water oxidation
Jiapeng Ji,
Yunpeng Hou,
Shiyu Zhou,
Tong Qiu,
Liang Zhang,
Lu Ma,
Chao Qian,
Shaodong Zhou,
Chengdu Liang,
Min Ling
Affiliations
Jiapeng Ji
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering Zhejiang University Hangzhou China
Yunpeng Hou
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering Zhejiang University Hangzhou China
Shiyu Zhou
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering Zhejiang University Hangzhou China
Tong Qiu
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering Zhejiang University Hangzhou China
Liang Zhang
Jiangsu Key Laboratory for Carbon‐Based Functional Materials & Devices, Joint International Research Laboratory of Carbon‐Based Functional Materials and Devices, Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Suzhou Jiangsu China
Lu Ma
National Synchrotron Light Source II, Brookhaven National Laboratory Upton New York USA
Chao Qian
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering Zhejiang University Hangzhou China
Shaodong Zhou
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering Zhejiang University Hangzhou China
Chengdu Liang
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering Zhejiang University Hangzhou China
Min Ling
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering Zhejiang University Hangzhou China
Abstract The oxygen evolution reaction (OER) activity of single‐atom catalysts (SACs) is closely related to the coordination environment of the active site. Oxygen‐coordinated atomic metal species bring about unique features beyond nitrogen‐coordinated atomic metal species due to the fact that the M–O bond is weaker than the M–N bond. Herein, a series of metal–oxygen–carbon structured low‐nucleus clusters (LNCs) are successfully anchored on the surface of multiwalled carbon nanotubes (M‐MWCNTs, M = Ni, Co, or Fe) through a foolproof low‐temperature gas transfer (300°C) method without any further treatment. The morphology and coordination configuration of the LNCs at the atomic level were confirmed by comprehensive characterizations. The synthetic Ni‐MWCNTs electrocatalyst features excellent OER activity and stability under alkaline conditions, transcending the performances of Co‐MWCNTs, Fe‐MWCNTs and RuO2. Density functional theory calculations reveal that the moderate oxidation of low‐nucleus Ni clusters changes the unoccupied orbital of Ni atoms, thereby lowering the energy barrier of the OER rate‐limiting step and making the OER process more energy‐efficient. This study demonstrates a novel versatile platform for large‐scale manufacturing of oxygen‐coordinated LNC catalysts.
