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Coexisting Single-Atomic Fe and Ni Sites on Hierarchically Ordered Porous Carbon as a Highly Efficient ORR Electrocatalyst |
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| Authors: | Zhengju Zhu Huajie Yin Yun Wang Cheng-Hao Chuang Lei Xing Mengyang Dong Ying-Rui Lu Gilberto Casillas-Garcia Yonglong Zheng Shan Chen Yuhai Dou Porun Liu Qilin Cheng Huijun Zhao |
| Affiliation: | 1. Centre for Clean Environment and Energy, Griffith University, Gold Coast, Queensland, 4222 Australia
Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science & Technology, Shanghai, 200237 China;2. Centre for Clean Environment and Energy, Griffith University, Gold Coast, Queensland, 4222 Australia;3. Department of Physics, Tamkang University, Tamsui 251, New Taipei City, 251301 Taiwan;4. Department of Engineering Science, University of Oxford, Oxford, OX1 3PJ UK;5. National Synchrotron Radiation Research Center, Hsinchu, 300 Taiwan;6. Electron Microscopy Center, University of Wollongong, Wollongong, NSW, 2500 Australia;7. Institute of Advanced Synthesis, School of Chemistry and Molecular Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials, Nanjing Tech University, 30 Puzhu South Road, Nanjing, 211816 China;8. Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science & Technology, Shanghai, 200237 China |
| Abstract: | The development of oxygen reduction reaction (ORR) electrocatalysts based on earth-abundant nonprecious materials is critically important for sustainable large-scale applications of fuel cells and metal–air batteries. Herein, a hetero-single-atom (h-SA) ORR electrocatalyst is presented, which has atomically dispersed Fe and Ni coanchored to a microsized nitrogen-doped graphitic carbon support with unique trimodal-porous structure configured by highly ordered macropores interconnected through mesopores. Extended X-ray absorption fine structure spectra confirm that Fe- and Ni-SAs are affixed to the carbon support via Fe? N4 and Ni? N4 coordination bonds. The resultant Fe/Ni h-SA electrocatalyst exhibits an outstanding ORR activity, outperforming SA electrocatalysts with only Fe- or Ni-SAs, and the benchmark Pt/C. The obtained experimental results indicate that the achieved outstanding ORR performance results from the synergetic enhancement induced by the coexisting Fe? N4 and Ni? N4 sites, and the superior mass-transfer capability promoted by the trimodal-porous-structured carbon support. |
| Keywords: | electrocatalysis fuel cell hierarchically porous structure oxygen reduction reaction single atom catalyst |