•  
  •  
 
Nano Research

Article Title

Porphyrin-like Fe-N4 sites with sulfur adjustment on hierarchical porous carbon for different rate-determining steps in oxygen reduction reaction

Authors

Konglin Wu, Department of Chemistry, Tsinghua University, Beijing 100084, China College of Chemistry and Materials Science, Key Laboratory of Functional Molecular Solids, the Ministry of Education, Anhui Normal University, Wuhu 241002, China
Xin Chen, Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials, Department of Chemistry, University of Science and Technology Beijing, Beijing 100083, China
Shoujie Liu, Department of Chemistry, Tsinghua University, Beijing 100084, China College of Chemistry and Materials Science, Key Laboratory of Functional Molecular Solids, the Ministry of Education, Anhui Normal University, Wuhu 241002, China
Yuan Pan, Department of Chemistry, Tsinghua University, Beijing 100084, China
Weng-Chon Cheong, Department of Chemistry, Tsinghua University, Beijing 100084, China
Wei Zhu, Department of Chemistry, Tsinghua University, Beijing 100084, China
Xing Cao, Department of Chemistry, Tsinghua University, Beijing 100084, China
Rongan Shen, Department of Chemistry, Tsinghua University, Beijing 100084, China
Wenxing Chen, Department of Chemistry, Tsinghua University, Beijing 100084, China
Jun Luo, Center for Electron Microscopy, Tianjin University of Technology, Tianjin 300384, China
Wensheng Yan, National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China, Hefei 230029, China
Lirong Zheng, Beijing Synchrotron Radiation Facility (NSRF), Institute of High Energy Physics, Chinese Academy of Science, Beijing 100049, China
Zheng Chen, Department of Chemistry, Tsinghua University, Beijing 100084, China
Dingsheng Wang, Department of Chemistry, Tsinghua University, Beijing 100084, China
Qing Peng, Department of Chemistry, Tsinghua University, Beijing 100084, China
Chen Chen, Department of Chemistry, Tsinghua University, Beijing 100084, China
Yadong Li, Department of Chemistry, Tsinghua University, Beijing 100084, China

Keywords

single-atom catalyst, heteroatom codoping, porous materials, oxygen reduction, electrocatalysis

Abstract

ABSTRACT We developed a strategy based on coordination polymer to synthesize singleatom site Fe/N and S-codoped hierarchical porous carbon (Fe1/N,S-PC). The as-obtained Fe1/N,S-PC exhibited superior oxygen reduction reaction (ORR) performance with a half-wave potential (E1/2, 0.904 V vs. RHE) that was better than that of commercial Pt/C (E1/2, 0.86 V vs. RHE), single-atom site Fe/N-doped hierarchical porous carbon (Fe1/N-PC) without S-doped (E1/2, 0.85 V vs. RHE), and many other nonprecious metal catalysts in alkaline medium. Moreover, the Fe1/N,S-PC revealed high methanol tolerance and firm stability. The excellent electrocatalytic activity of Fe1/N,S-PC is attributed to the synergistic effects from the atomically dispersed porphyrin-like Fe-N4 active sites, the heteroatom codoping (N and S), and the hierarchical porous structure in the carbon materials. The calculation based on density functional theory further indicates that the catalytic performance of Fe1/N,S-PC is better than that of Fe1/N-PC owing to the sulfur doping that yielded different rate-determining steps.

Graphical Abstract

Publisher

Tsinghua University Press

Share

COinS