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Electronic Spin Moment As a Catalytic Descriptor for Fe Single-Atom Catalysts Supported on C2N.

  • Zhong, Wenhui1, 2
  • Qiu, Yue3
  • Shen, Hujun4
  • Wang, Xijun5
  • Yuan, Jianyong6
  • Jia, Chuanyi4
  • Bi, Siwei1
  • Jiang, Jun5
  • 1 School of Chemistry and Chemical Engineering, Qufu Normal University, Qufu, Shandong 273165, P. R. China. , (China)
  • 2 Gusu Laboratory of Materials, Suzhou, Jiangsu 215123, P. R. China. , (China)
  • 3 Grimwade Centre for Cultural Materials Conservation, School of Historical and Philosophical Studies, Faculty of Arts University of Melbourne, Parkville, VIC 3052, Australia. , (Australia)
  • 4 Guizhou Provincial Key Laboratory of Computational Nano-Material Science, Guizhou Education University, Guiyang, Guizhou 550018, P. R. China. , (China)
  • 5 Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China. , (China)
  • 6 Otsuka Material Science and Technology (Shanghai) Co., Ltd., Shanghai 200233, P. R. China. , (China)
Published Article
Journal of the American Chemical Society
American Chemical Society
Publication Date
Mar 11, 2021
DOI: 10.1021/jacs.1c00889
PMID: 33705130


The electrocatalytic activity of transition-metal-based compounds is strongly related to the spin states. However, the underlying relationship connecting spin to catalytic activity remains unclear. Herein, we carried out density functional theory calculations on oxygen reduction reaction (ORR) catalyzed by Fe single-atom supported on C2N (C2N-Fe) to shed light on this relationship. It is found that the change of electronic spin moments of Fe and O2 due to molecular-catalyst adsorption scales with the amount of electron transfer from Fe to O2, which promotes the catalytic activity of C2N-Fe for driving ORR. The nearly linear relationship between the catalytic activity and spin moment variation suggests electronic spin moment as a promising catalytic descriptor for Fe single-atom based catalysts. Following the revealed relationship, the ORR barrier on C2N-Fe was tuned to be as low as 0.10 eV through judicious manipulation of spin states. These findings thus provide important insights into the relationship between catalytic activity and spin, leading to new strategies for designing transition metal single-atom catalysts.

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