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Research Article

Coordinatively unsaturated single Co atoms immobilized on C2N for efficient oxygen reduction reaction

Wenjing Xu1,2,§, Yidong Sun3,§, Jiaqi Zhou4, Maoqi Cao2( ), Jun Luo2, Haili Mao2, Pengfei Hu5,6, Hongfei Gu1, Huazhang Zhai1, Huishan Shang1,4( ), Zhi Cai5( )
Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Key Laboratory of Efficient and Comprehensive Utilization of Biomass-based Agricultural and Forestry Wastes of Qiannan, Qiannan Normal University for Nationalities, Duyun 558000, China
School of Physics and Technology, and MOE Key Laboratory of Artificial Micro- and Nano-structures, Wuhan University, Wuhan 430072, China
School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China
School of Physics, Beihang University, Beijing 100191, China
Research Institute of Aero-Engine, Beihang University, Beijing 102206, China

§ Wenjing Xu and Yidong Sun contributed equally to this work.

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Graphical Abstract

Surprising catalytic activity can be obtained by anchoring metal single atoms through C2N supports with unique regular structures. The loading of Co metal atoms on C2N materials was designed for electrocatalytic oxygen reduction reaction (ORR) to H2O. The catalytic activity of CoSA-C2N catalysts with Co-N2 active sites is higher than that of C2N catalysts. This work provides a novel and efficient single-atom catalyst for ORR.

Abstract

Developing cost-effective and high-efficiency oxygen reduction reaction (ORR) catalysts is imperative for promoting the substantial progress of fuel cells and metal-air batteries. The coordination and geometric engineering of single-atom catalysts (SACs) occurred the promising approach to overcome the thermodynamics and kinetics problems in high-efficiency electrocatalysis. Herein, we rationally constructed atomically dispersed Co atoms on porous N-enriched graphene material C2N (CoSA-C2N) for efficient oxygen reduction reaction (ORR). Systematic characterizations demonstrated the active sites for CoSA-C2N is as identified as coordinatively unsaturated Co-N2 moiety, which exhibits ORR intrinsic activity. Structurally, the porous N-enriched graphene framework in C2N could effectively increase the accessibility to the active sites and promote mass transfer rate, contributing to improved ORR kinetics. Consequently, CoSA-C2N exhibited superior ORR performance in both acidic and alkaline conditions as well as impressive long-term durability. The coordination and geometric engineering of SACs will provide a novel approach to advanced catalysts for energy related applications.

Keywords

single-atom catalystsunsaturated coordinationgeometric engineeringoxygen reduction reactionporous graphene nitride

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Nano Research
Volume 16 Issue 2,
February 2023
Pages 2294-2301
DOI: 10.1007/s12274-022-5212-7
Cite this article:
Xu W, Sun Y, Zhou J, et al. Coordinatively unsaturated single Co atoms immobilized on C2N for efficient oxygen reduction reaction. Nano Research, 2023, 16(2): 2294-2301. https://doi.org/10.1007/s12274-022-5212-7
Topics:
Oxygen evolution reaction

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Received: 09 September 2022
Revised: 12 October 2022
Accepted: 15 October 2022
Published: 23 November 2022
© Tsinghua University Press 2022
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