An Adjacent Atomic Platinum Site Enables Single-Atom Iron with High Oxygen Reduction Reaction Performance

被引：351

作者：

Han, Ali ^{[1
]}

Wang, Xijun ^{[2
]}

Tang, Kun ^{[3
]}

Zhang, Zedong ^{[1
]}

Ye, Chenliang ^{[1
]}

Kong, Kejian ^{[1
]}

Hu, Haibo ^{[3
]}

Zheng, Lirong ^{[4
]}

Jiang, Peng ^{[1
]}

Zhao, Changxin ^{[5
]}

Zhang, Qiang ^{[5
]}

Wang, Dingsheng ^{[1
]}

Li, Yadong ^{[1
]}

机构：

[1] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

[2] Univ Sci & Technol China, Sch Chem & Mat Sci, CAS Ctr Excellence Nanosci, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China

[3] Anhui Univ, Sch Phys & Mat Sci, Hefei 230601, Peoples R China

[4] Chinese Acad Sci, Beijing Synchrotron Radiat Facil Inst High Energy, 19 Yuquan Rd, Beijing 100049, Peoples R China

[5] Tsinghua Univ, Beijing Key Lab Green Chem React Engn & Technol, Dept Chem Engn, Beijing 100084, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2021年 / 60卷 / 35期

基金：

中国国家自然科学基金; 国家重点研发计划;

关键词：

dual atomic sites; modulation effect; oxygen reduction reaction; platinum; single-atom catalysts; DOPED CARBON; CATALYSTS; ELECTROCATALYSTS; COBALT; MODEL;

D O I：

10.1002/anie.202105186

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The modulation effect has been widely investigated to tune the electronic state of single-atomic M-N-C catalysts to enhance the activity of oxygen reduction reaction (ORR). However, the in-depth study of modulation effect is rarely reported for the isolated dual-atomic metal sites. Now, the catalytic activities of Fe-N-4 moiety can be enhanced by the adjacent Pt-N-4 moiety through the modulation effect, in which the Pt-N-4 acts as the modulator to tune the 3d electronic orbitals of Fe-N-4 active site and optimize ORR activity. Inspired by this principle, we design and synthesize the electrocatalyst that comprises isolated Fe-N-4/Pt-N-4 moieties dispersed in the nitrogen-doped carbon matrix (Fe-N-4/Pt-N-4@NC) and exhibits a half-wave potential of 0.93 V vs. RHE and negligible activity degradation (Delta E-1/2 = 8 mV) after 10000 cycles in 0.1 M KOH. We also demonstrate that the modulation effect is not effective for optimizing the ORR performances of Co-N-4/Pt-N-4 and Mn-N-4/Pt-N-4 systems.

引用

页码：19262 / 19271

页数：10

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