•  
  •  
 
Nano Research

Article Title

Fe atoms anchored on defective nitrogen doped hollow carbon spheres as efficient electrocatalysts for oxygen reduction reaction

Authors

Panpan Su, College of Mathematics and Physics, Shanghai University of Electric Power, Shanghai 200090, China;State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Wenjuan Huang, College of Mathematics and Physics, Shanghai University of Electric Power, Shanghai 200090, China;State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Jiangwei Zhang, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Utsab Guharoy, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;State Key Laboratory of Radiation Medicine and Protection, Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, School for Radiological and Interdisciplinary Sciences, Soochow University, Suzhou 215123, China
Qinggang Du, College of Mathematics and Physics, Shanghai University of Electric Power, Shanghai 200090, China;State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Qiao Sun, State Key Laboratory of Radiation Medicine and Protection, Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, School for Radiological and Interdisciplinary Sciences, Soochow University, Suzhou 215123, China
Qike Jiang, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;Division of Energy Research Resources, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Yi Cheng, Department of Environmental Engineering, School of Metallurgy and Environment, Central South University, Changsha 410083, China;WA School of Mines: Minerals, Energy and Chemical Engineering, Curtin University, Perth, WA 6102, Australia
Jie Yang, College of Mathematics and Physics, Shanghai University of Electric Power, Shanghai 200090, China
Xiaoli Zhang, State Centre for International Cooperation on Designer Low-Carbon & Environmental Materials, School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
Yongsheng Liu, College of Mathematics and Physics, Shanghai University of Electric Power, Shanghai 200090, China
San Ping Jiang, WA School of Mines: Minerals, Energy and Chemical Engineering, Curtin University, Perth, WA 6102, Australia
Jian Liu, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;WA School of Mines: Minerals, Energy and Chemical Engineering, Curtin University, Perth, WA 6102, Australia;DICP-Surrey Joint Centre for Future Materials, Department of Chemical and Process Engineering, University of Surrey, Guildford, Surrey, UK

Keywords

atomic iron, nitrogen defect, coordination environment, hollow carbon spheres, oxygen reduction reaction

Abstract

Defective electrocatalysts, especially for intrinsic defective carbon, have aroused a wide concern owing to high spin and charge densities. However, the designated nitrogen species favorable for creating defects by the removal of nitrogen, and the influence of defects for the coordination structure of active site and oxygen reduction reaction (ORR) activity have not been elucidated. Herein, we designed and synthesized a pair of electrocatalysts, denoted as Fe-N/C and Fe-ND/C for coordination sites of atomic iron-nitrogen and iron-nitrogen/defect configuration embedded in hollow carbon spheres, respectively, through direct pyrolysis of their corresponding hollow carbon spheres adsorbed with Fe(acac)3. The nitrogen defects were fabricated via the evaporation of pyrrolic-N on nitrogen doped hollow carbon spheres. Results of comparative experiments between Fe-N/C and Fe-ND/C reveal that Fe-ND/C shows superior ORR activity with an onset potential of 30 mV higher than that of Fe-N/C. Fe-ND sites are more favorable for the enhancement of ORR activity. Density functional theory (DFT) calculation demonstrates that Fe-ND/C with proposed coordination structure of FeN4−x (0

Publisher

Tsinghua University Press

Share

COinS