Secondary-Atom-Doping Enables Robust Fe\u2013N\u2013C Single-Atom Catalysts with Enhanced Oxygen Reduction Reaction

Xin Luo,Hengjia Wang,Xiao Zhao,Xiaoqian Wei,Wenling Gu,Takuma Kaneko,Yusuke Yoshida,Chengzhou Zhu

doi:10.1007/s40820-020-00502-5

Xin Luo, Hengjia Wang + Show 6 more

Open Access

https://doi.org/10.1007/s40820-020-00502-5

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Abstract

HighlightsSecondary-atom-doped strategy was proposed to synthesize single-atom electrocatalyst.The increase in both the density of active sites and their intrinsic activity was achieved simultaneously.The resultant single-atom catalyst shows outstanding ORR activity in acidic media.

Highlights

Tremendous efforts have been devoted to the exploration of environment-friendly and sustainable energy conversion [1,2,3,4]
Pt-based catalysts with superior activity are promising electrocatalysts for the oxygen reduction reaction (ORR) [9,10,11,12]. Their inhibitive cost, scarcity and instability call for nonprecious metal catalysts (NPMCs) that have the advantages of natural abundance and low cost [13,14,15,16,17]
Experimental results and density functional theory (DFT) calculations manifest that the outstanding ORR performance of the catalyst is significantly correlated with tuning the density and coordination environment of active sites

Summary

Introduction

Tremendous efforts have been devoted to the exploration of environment-friendly and sustainable energy conversion [1,2,3,4]. Pt-based catalysts with superior activity are promising electrocatalysts for the ORR [9,10,11,12] Their inhibitive cost, scarcity and instability call for nonprecious metal catalysts (NPMCs) that have the advantages of natural abundance and low cost [13,14,15,16,17]. To achieve atomic dispersion of metal atoms, SACs usually have a very low density of metal sites that limits catalytic performance in practical devices To overcome these limitations of SACs, several strategies have been developed to improve catalytic activity [29,30,31,32,33,34,35,36]. The as-synthesized Fe–N–C/FeN possesses a remarkable electrocatalytic activity in acidic solution with the remarkable onset potential (Eonset, 0.85 V) and half-wave potential (E1/2, 0.81 V) and high stability with scarcely any decay in E1/2 after 30,000 cycles, which exhibit comparable activity but superior stability relative to commercial Pt/C

Physical Characterizations

Materials Preparation

Electrochemical Experiments

Materials Characterizations

Electrochemical Measurements

Conclusions