The Difference Se Makes: A Bio-Inspired Dppf-Supported Nickel Selenolate Complex Boosts Dihydrogen Evolution with High Oxygen Tolerance
| Autor: | Quan-Feng He, Ji-Huai Wu, Yunwen Tao, Li-Ping Cheng, Jinqing Lin, Dan Tian, Zhanhua Wei, Geng-Geng Luo, Qichun Zhang, Zhong-Hua Pan, Qiao-Yu Wu, Di Sun |
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| Přispěvatelé: | School of Materials Science & Engineering |
| Rok vydání: | 2018 |
| Předmět: |
inorganic chemicals
Materials [Engineering] Proton 010405 organic chemistry Organic Chemistry chemistry.chemical_element General Chemistry 010402 general chemistry Electrochemistry Electrocatalyst 01 natural sciences Combinatorial chemistry Catalysis Dihydrogen Evolution 0104 chemical sciences Metal chemistry.chemical_compound Nickel chemistry Ferrocene visual_art visual_art.visual_art_medium DFT Calculations Selenium |
| Zdroj: | Chemistry (Weinheim an der Bergstrasse, Germany). 24(33) |
| ISSN: | 1521-3765 |
| Popis: | Inspired by the metal active sites of [NiFeSe]-hydrogenases, a dppf-supported nickel(II) selenolate complex (dppf=1,1'-bis(diphenylphosphino)ferrocene) shows high catalytic activity for electrochemical proton reduction with a remarkable enzyme-like H2 evolution turnover frequency (TOF) of 7838 s-1 under an Ar atmosphere, which markedly surpasses the activity of a dppf-supported nickel(II) thiolate analogue with a low TOF of 600 s-1 . A combined study of electrochemical experiments and DFT calculations shed light on the catalytic process, suggesting that selenium atom as a bio-inspired proton relay plays a key role in proton exchange and enhancing catalytic activity of H2 production. For the first time, this type of Ni selenolate-containing electrocatalyst displays a high degree of O2 and H2 tolerance. Our results should encourage the development of the design of highly efficient oxygen-tolerant Ni selenolate molecular catalysts. |
| Databáze: | OpenAIRE |
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