Turning on Zn 4s Electrons in a N 2 ‐Zn‐B 2 Configuration to Stimulate Remarkable ORR Performance
| Autor: | Jing Zhang, Yongfeng Hu, Jing Wang, Jiujun Zhang, Hongguan Li, Shuhu Liu, Yanglong Hou, Meirong Xia, Yufeng Zhao, John S. Tse |
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| Rok vydání: | 2020 |
| Předmět: |
Materials science
010405 organic chemistry Inorganic chemistry chemistry.chemical_element General Chemistry Reaction intermediate Zinc Electron 010402 general chemistry Electrocatalyst 01 natural sciences Catalysis Oxygen reduction 0104 chemical sciences Delocalized electron chemistry Electron configuration |
| Zdroj: | Angewandte Chemie International Edition. 60:181-185 |
| ISSN: | 1521-3773 1433-7851 |
| DOI: | 10.1002/anie.202009991 |
| Popis: | A zinc-based single-atom catalyst has been recently explored with distinguished stability, of which the fully occupied Zn2+ 3d10 electronic configuration is Fenton-reaction-inactive, but the catalytic activity is thus inferior. Herein, we report an approach to manipulate the s-band by constructing a B,N co-coordinated Zn-B/N-C catalyst. We confirm both experimentally and theoretically that the unique N2 -Zn-B2 configuration is crucial, in which Zn+ (3d10 4s1 ) can hold enough delocalized electrons to generate suitable binding strength for key reaction intermediates and promote the charge transfer between catalytic surface and ORR reactants. This exclusive effect is not found in the other transition-metal counterparts such as M-B/N-C (M=Mn, Fe, Co, Ni and Cu). Consequently, the as-obtained catalyst demonstrates impressive ORR activity, along with remarkable long-term stability in both alkaline and acid media. This work presents a new concept in the further design of electrocatalyst. |
| Databáze: | OpenAIRE |
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