Volume 19, Issue 44 2301327
Research Article

Atomic Engineering Modulates Oxygen Reduction of Hollow Carbon Matrix Confined Single Metal-Nitrogen Sites for Zinc-Air Batteries

Haihua Wu

Haihua Wu

State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014 China

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Xin Xu

Xin Xu

State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014 China

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Jiahao Wu

Jiahao Wu

State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014 China

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Juanjuan Zhai

Juanjuan Zhai

State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014 China

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Feng Wu

Feng Wu

State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014 China

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Yudan Li

Yudan Li

State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014 China

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Sen Jiang

Sen Jiang

State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014 China

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Jiangwei Zhang

Corresponding Author

Jiangwei Zhang

Science Center of Energy Material and Chemistry, College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot, Inner Mongolia, 010021 China

E-mail: [email protected]; [email protected]; [email protected]

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Haobo Li

Corresponding Author

Haobo Li

School of Chemical Engineering, The University of Adelaide, Adelaide, South Australia, 5005 Australia

E-mail: [email protected]; [email protected]; [email protected]

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Yunfang Gao

Corresponding Author

Yunfang Gao

State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014 China

E-mail: [email protected]; [email protected]; [email protected]

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First published: 07 July 2023
Citations: 16

Abstract

The systematical understanding of metal-dependent activity in electrocatalyzing oxygen reduction reaction (ORR), a vital reaction with sluggish kinetics for zinc-air batteries, remains quite unclear. An atomic and spatial engineering modulating ORR activity over hollow carbon quasi-sphere (HCS) confined in a series of single M-N (M = Cu, Mn, Ni) sites is reported here. Based on the theoretical prediction and experimental validation, Cu-N4 site with the lowest overpotential shows a better ORR kinetics than Mn-N4 and Ni-N4. The ORR activity of single-atom Cu center can be further improved by decreasing the coordination number of N to two, namely Cu-N2, due to the enhancement of electrons with lower coordination structure. Benefitting from the unique spatial confinement effect of the HCS structure in modulating electronic feature of active sites, the Cu-N2 site confined in HCS also delivers highly improved ORR kinetics and activity relative to that on planner graphene. Additionally, the best catalyst holds excellent promise in the application of zinc-air batteries. The findings will pave a new way to atomically and electronically tune active sites with high efficiency for other single-atom catalysts.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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