Understanding the Synergistic Effects of Cobalt Single Atoms and Small Nanoparticles: Enhancing Oxygen Reduction Reaction Catalytic Activity and Stability for Zinc‐Air Batteries

Advanced Functional Materials - Tập 31 Số 45 - 2021
Zhe Wang1, Chao Zhu1, Hua Tan2, Jan Liu1, Lulu Xu1, Yongqi Zhang3,4, Yipu Liu5,6, Xiaoxin Zou5, Zheng Liu7,8,1, Xuehong Lu1
1School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore
2School of Physical and Mathematical Sciences, Nanyang Technological University 21 Nanyang Link, Singapore 637371, Singapore
3Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China
4Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313002, China
5State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, Jilin 130012, China
6State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou 570228, P. R. China
7CINTRA CNRS/NTU/THALES, UMI 3288, Research Techno Plaza, 50 Nanyang Drive, Border X Block, Level 6, Singapore 637553, Singapore
8School of Electrical and Electronic Engineering, Nanyang Technological University, Singapore 639798, Singapore

Tóm tắt

AbstractThe development of earth‐abundant oxygen reduction reaction (ORR) catalysts with high catalytic activity and good stability for practical metal‐air batteries remains an enormous challenge. Herein, a highly efficient and durable ORR catalyst is reported, which consists of atomically dispersed Co single atoms (Co‐SAs) in the form of Co‐N4 moieties and small Co nanoparticles (Co‐SNPs) co‐anchored on nitrogen‐doped porous carbon nanocage (Co‐SAs/SNPs@NC). Benefiting from the synergistic effect of Co‐SAs and Co‐SNPs as well as the enhanced anticorrosion capability of the carbon matrix brought by its improved graphitization degree, the resultant Co‐SAs/SNPs@NC catalyst exhibits outstanding ORR activity and remarkable stability in alkaline media, outperforming Co‐SAs‐based catalyst (Co‐SAs@NC), and benchmark Pt/C catalyst. Density functional theory calculations reveal that the strong interaction between Co‐SNPs and Co‐N4 sites can increase the valence state of the active Co atoms in Co‐SAs/SNPs@NC and moderate the adsorption free energy of ORR intermediates, thus facilitating the reduction of O2. Moreover, the practical zinc‐air battery assembled with Co‐SAs/SNPs@NC catalyst demonstrates a maximum power density of 223.5 mW cm–2, a high specific capacity of 742 W h kg–1 at 50 mA cm–2 and a superior cycling stability.

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Advanced Functional Materials

Tập 31 Số 45

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