Boosting Oxygen Reduction Reaction Performance of Fe Single-Atom Catalysts Via Precise Control of the Coordination Environment

被引：1

作者：

Zhang, Shiyu ^{[1
]}

Sun, Buwei ^{[2
]}

Liao, Kang ^{[1
]}

Wang, Xin ^{[1
]}

Chen, Zanyu ^{[1
]}

Wang, Jiajun ^{[1
]}

Hu, Wenbin ^{[1
]}

Han, Xiaopeng ^{[1
]}

机构：

[1] Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ,State Key Lab Precious Met Funct Mat,N, Tianjin 300350, Peoples R China

[2] Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou 350207, Peoples R China

来源：

ADVANCED FUNCTIONAL MATERIALS | 2025年

基金：

中国国家自然科学基金;

关键词：

coordination shell; heterogeneous atom; oxygen reduction; precise local structure; single atom; DESIGN;

D O I：

10.1002/adfm.202425640

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Fe single-atom on N-doped carbon (FeN-C) catalysts emerge as promising alternatives to commercial Pt/C for the oxygen reduction reaction. Heterogeneous atom doping is proposed to be effective for modulating catalyst performance. Despite this, the relationship between the fine coordination structure of the doped atoms and catalytic activity of the central metal site remains poorly understood. Herein, Fe single-atom catalysts with S doped in either the first coordination shell (FeSN-C) or the second coordination shell (FeN-SC) of the Fe active site are synthesized to compare the effects of different coordination structure. FeN-SC exhibits prominent performance with a half-wave potential of 0.92 V in rotating disk electrode and a peak power density of 251 mW cm(-2) in the zinc-air battery. Theoretical studies reveal that S doping effectively modulates the electronic structure and charge transfer at the Fe center. Compared to S atoms directly coordinated within the first coordination shell, S located in the second coordination shell is more effective in optimizing the adsorption and desorption energy barriers of oxygen-containing intermediates at the active sites. This study provides a new strategy to adjust the catalytic performance by engineering the multilayer coordination structure at the active center of the single-atom catalyst.

引用

页数：10

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