Salt Effect Engineering Single Fe‐N2P2‐Cl Sites on Interlinked Porous Carbon Nanosheets for Superior Oxygen Reduction Reaction and Zn‐Air Batteries

Author:

Tan Xiaojie1,Zhang Jinqiang2,Cao Fengliang1,Liu Yachao1,Yang Hao1,Zhou Qiang1,Li Xudong1,Wang Rui1,Li Zhongtao1,Hu Han1,Zhao Qingshan1,Wu Mingbo1ORCID

Affiliation:

1. State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical Engineering College of New Energy China University of Petroleum (East China) Qingdao 266580 China

2. School of Chemical Engineering and Advanced Materials The University of Adelaide Adelaide SA 5005 Australia

Abstract

AbstractDeveloping efficient metal‐nitrogen‐carbon (M‐N‐C) single‐atom catalysts for oxygen reduction reaction (ORR) is significant for the widespread implementation of Zn‐air batteries, while the synergic design of the matrix microstructure and coordination environment of metal centers remains challenges. Herein, a novel salt effect‐induced strategy is proposed to engineer N and P coordinated atomically dispersed Fe atoms with extra‐axial Cl on interlinked porous carbon nanosheets, achieving a superior single‐atom Fe catalyst (denoted as Fe‐NP‐Cl‐C) for ORR and Zn‐air batteries. The hierarchical porous nanosheet architecture can provide rapid mass/electron transfer channels and facilitate the exposure of active sites. Experiments and density functional theory (DFT) calculations reveal the distinctive Fe‐N2P2‐Cl active sites afford significantly reduced energy barriers and promoted reaction kinetics for ORR. Consequently, the Fe‐NP‐Cl‐C catalyst exhibits distinguished ORR performance with a half‐wave potential (E1/2) of 0.92 V and excellent stability. Remarkably, the assembled Zn‐air battery based on Fe‐NP‐Cl‐C delivers an extremely high peak power density of 260 mW cm−2 and a large specific capacity of 812 mA h g−1, outperforming the commercial Pt/C and most reported congeneric catalysts. This study offers a new perspective on structural optimization and coordination engineering of single‐atom catalysts for efficient oxygen electrocatalysis and energy conversion devices.

Funder

National Natural Science Foundation of China

Major Scientific and Technological Innovation Project of Shandong Province

Taishan Scholar Project of Shandong Province

Natural Science Foundation of Shandong Province

National Key Research and Development Program of China

Publisher

Wiley

Subject

General Physics and Astronomy,General Engineering,Biochemistry, Genetics and Molecular Biology (miscellaneous),General Materials Science,General Chemical Engineering,Medicine (miscellaneous)

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