Fe atoms anchored on defective nitrogen doped hollow carbon spheres as efficient electrocatalysts for oxygen reduction r
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ge 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 3 Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China 4 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 5 Division of Energy Research Resources, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China 6 Department of Environmental Engineering, School of Metallurgy and Environment, Central South University, Changsha 410083, China 7 WA School of Mines: Minerals, Energy and Chemical Engineering, Curtin University, Perth, WA 6102, Australia 8 State Centre for International Cooperation on Designer Low-Carbon & Environmental Materials, School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China 9 DICP-Surrey Joint Centre for Future Materials, Department of Chemical and Process Engineering, University of Surrey, Guildford, Surrey, UK § Panpan Su, Wenjuan Huang, and Jiangwei Zhang contributed equally to this work. 2
© The Author(s) 2020 Received: 24 June 2020 / Revised: 22 September 2020 / Accepted: 30 September 2020
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
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