Edge-Rich Fe-N4 Active Sites in Defective Carbon for Oxygen Reduction Catalysis

Advanced Materials
Xin WangXiangdong Yao

Abstract

Controllably constructing nitrogen-modified divacancies (ND) in carbon substrates to immobilize atomic Fe species and unveiling the advantageous configuration is still challenging, but indispensable for attaining optimal Fe-N-C catalysts for the oxygen reduction reaction (ORR). Herein, a fundamental investigation of unfolding intrinsically superior edge-ND trapped atomic Fe motifs (e-ND-Fe) relative to an intact center model (c-ND-Fe) in ORR electrocatalysis is reported. Density functional theory calculations reveal that local electronic redistribution and bandgap shrinkage for e-ND-Fe endow it with a lower free-energy barrier toward direct four-electron ORR. Inspired by this, a series of atomic Fe catalysts with adjustable ND-Fe coordination are synthesized, which verify that ORR performance highly depends on the concentration of e-ND-Fe species. Remarkably, the best e-ND-Fe catalyst delivers a favorable kinetic current density and halfwave potential that can be comparable to benchmark Pt-C under acidic conditions. This work will guide to develop highly active atomic metal catalysts through rational defect engineering.

References

Apr 4, 2009·Science·Hubert A Gasteiger, Nenad M Marković
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Sep 1, 2015·Angewandte Chemie·Chang Hyuck ChoiKarl J J Mayrhofer
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Feb 20, 2019·Advanced Materials·Yuyan ShaoPiotr Zelenay
Mar 6, 2019·Journal of the American Chemical Society·Yunteng QuYadong Li
Mar 26, 2019·Advanced Materials·Yichao LinLiang Chen
Jun 15, 2019·Nature Communications·Feng LiJong-Beom Baek

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Citations

Jul 16, 2020·Advanced Materials·Hui ChenXiaoxin Zou
Sep 15, 2020·Chemical Communications : Chem Comm·Jiawei ShiWeiwei Cai
Dec 29, 2020·Chemical Communications : Chem Comm·Jiawei ShiWeiwei Cai
Sep 24, 2021·Journal of the American Chemical Society·Xin ZhaoYingwei Li

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