The difference Se makes : a bio-inspired dppf-supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance
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 ...
| Main Authors: | , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
| Published: |
2020
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/139416 |
| _version_ | 1811683842188115968 |
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| author | Pan, Zhong-Hua Tao, Yun-Wen He, Quan-Feng Wu, Qiao-Yu Cheng, Li-Ping Wei, Zhan-Hua Wu, Ji-Huai Lin, Jin-Qing Sun, Di Zhang, Qi-Chun Tian, Dan Luo, Geng-Geng |
| author2 | School of Materials Science & Engineering |
| author_facet | School of Materials Science & Engineering Pan, Zhong-Hua Tao, Yun-Wen He, Quan-Feng Wu, Qiao-Yu Cheng, Li-Ping Wei, Zhan-Hua Wu, Ji-Huai Lin, Jin-Qing Sun, Di Zhang, Qi-Chun Tian, Dan Luo, Geng-Geng |
| author_sort | Pan, Zhong-Hua |
| collection | NTU |
| description | 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. |
| first_indexed | 2024-10-01T04:19:09Z |
| format | Journal Article |
| id | ntu-10356/139416 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:19:09Z |
| publishDate | 2020 |
| record_format | dspace |
| spelling | ntu-10356/1394162020-06-01T10:01:49Z The difference Se makes : a bio-inspired dppf-supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance Pan, Zhong-Hua Tao, Yun-Wen He, Quan-Feng Wu, Qiao-Yu Cheng, Li-Ping Wei, Zhan-Hua Wu, Ji-Huai Lin, Jin-Qing Sun, Di Zhang, Qi-Chun Tian, Dan Luo, Geng-Geng School of Materials Science & Engineering Engineering::Materials DFT Calculations Dihydrogen Evolution 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. 2020-05-19T07:21:39Z 2020-05-19T07:21:39Z 2018 Journal Article Pan, Z.-H., Tao, Y.-W., He, Q.-F., Wu, Q.-Y., Cheng, L.-P., Wei, Z.-H., . . . Luo, G.-G. (2018). The difference Se makes : a bio-inspired dppf-supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance. Chemistry - A European Journal, 24(33), 8275-8280. doi:10.1002/chem.201801893 0947-6539 https://hdl.handle.net/10356/139416 10.1002/chem.201801893 29694691 2-s2.0-85047666350 33 24 8275 8280 en Chemistry - A European Journal This is the accepted version of the following article: Pan, Z.-H., Tao, Y.-W., He, Q.-F., Wu, Q.-Y., Cheng, L.-P., Wei, Z.-H., . . . Luo, G.-G. (2018). The difference Se makes : a bio-inspired dppf-supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance. Chemistry - A European Journal, 24(33), 8275-8280, which has been published in final form at dx.doi.org/10.1002/chem.201801893. This article may be used for non-commercial purposes in accordance with the Wiley Self-Archiving Policy [https://authorservices.wiley.com/authorresources/Journal-Authors/licensing/self-archiving.html]. |
| spellingShingle | Engineering::Materials DFT Calculations Dihydrogen Evolution Pan, Zhong-Hua Tao, Yun-Wen He, Quan-Feng Wu, Qiao-Yu Cheng, Li-Ping Wei, Zhan-Hua Wu, Ji-Huai Lin, Jin-Qing Sun, Di Zhang, Qi-Chun Tian, Dan Luo, Geng-Geng The difference Se makes : a bio-inspired dppf-supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance |
| title | The difference Se makes : a bio-inspired dppf-supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance |
| title_full | The difference Se makes : a bio-inspired dppf-supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance |
| title_fullStr | The difference Se makes : a bio-inspired dppf-supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance |
| title_full_unstemmed | The difference Se makes : a bio-inspired dppf-supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance |
| title_short | The difference Se makes : a bio-inspired dppf-supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance |
| title_sort | difference se makes a bio inspired dppf supported nickel selenolate complex boosts dihydrogen evolution with high oxygen tolerance |
| topic | Engineering::Materials DFT Calculations Dihydrogen Evolution |
| url | https://hdl.handle.net/10356/139416 |
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