The Difference Se Makes: A Bio-Inspired Dppf-Supported Nickel Selenolate Complex Boosts Dihydrogen Evolution with High Oxygen Tolerance

Zhong-Hua Pan; Yun-Wen Tao; Quan-Feng He; Qiao-Yu Wu; Li-Ping Cheng; Zhan-Hua Wei; Ji-Huai Wu; Jin-Qing Lin; Di Sun; Qi-Chun Zhang; Dan Tian; Geng-Geng Luo

doi:10.1002/chem.201801893

The Difference Se Makes: A Bio-Inspired Dppf-Supported Nickel Selenolate Complex Boosts Dihydrogen Evolution with High Oxygen Tolerance

Zhong-Hua Pan, Yun-Wen Tao, Quan-Feng He, Qiao-Yu Wu, Li-Ping Cheng, Zhan-Hua Wei, Ji-Huai Wu, Jin-Qing Lin, Di Sun, Qi-Chun Zhang^*, Dan Tian, Geng-Geng Luo^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

38 Citations (Scopus)

Abstract

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.

Original language	English
Pages (from-to)	8275-8280
Journal	Chemistry - A European Journal
Volume	24
Issue number	33
Online published	25 Apr 2018
DOIs	https://doi.org/10.1002/chem.201801893
Publication status	Published - 12 Jun 2018
Externally published	Yes

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This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Research Keywords

DFT calculations
dihydrogen evolution
molecular catalysis
nickel(II) complexes
oxygen tolerance

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10.1002/chem.201801893

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Pan, Z.-H., Tao, Y.-W., He, Q.-F., Wu, Q.-Y., Cheng, L.-P., Wei, Z.-H., Wu, J.-H., Lin, J.-Q., Sun, D., Zhang, Q.-C., Tian, D., & 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. https://doi.org/10.1002/chem.201801893

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title = "The Difference Se Makes: A Bio-Inspired Dppf-Supported Nickel Selenolate Complex Boosts Dihydrogen Evolution with High Oxygen Tolerance",

abstract = "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.",

keywords = "DFT calculations, dihydrogen evolution, molecular catalysis, nickel(II) complexes, oxygen tolerance, DFT calculations, dihydrogen evolution, molecular catalysis, nickel(II) complexes, oxygen tolerance, DFT calculations, dihydrogen evolution, molecular catalysis, nickel(II) complexes, oxygen tolerance",

author = "Zhong-Hua Pan and Yun-Wen Tao and Quan-Feng He and Qiao-Yu Wu and Li-Ping Cheng and Zhan-Hua Wei and Ji-Huai Wu and Jin-Qing Lin and Di Sun and Qi-Chun Zhang and Dan Tian and Geng-Geng Luo",

year = "2018",

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doi = "10.1002/chem.201801893",

language = "English",

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}

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 et al.
In: Chemistry - A European Journal, Vol. 24, No. 33, 12.06.2018, p. 8275-8280.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - The Difference Se Makes

T2 - A Bio-Inspired Dppf-Supported Nickel Selenolate Complex Boosts Dihydrogen Evolution with High Oxygen Tolerance

AU - Pan, Zhong-Hua

AU - Tao, Yun-Wen

AU - He, Quan-Feng

AU - Wu, Qiao-Yu

AU - Cheng, Li-Ping

AU - Wei, Zhan-Hua

AU - Wu, Ji-Huai

AU - Lin, Jin-Qing

AU - Sun, Di

AU - Zhang, Qi-Chun

AU - Tian, Dan

AU - Luo, Geng-Geng

PY - 2018/6/12

Y1 - 2018/6/12

N2 - 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.

AB - 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.

KW - DFT calculations

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KW - molecular catalysis

KW - nickel(II) complexes

KW - oxygen tolerance

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KW - dihydrogen evolution

KW - molecular catalysis

KW - nickel(II) complexes

KW - oxygen tolerance

KW - DFT calculations

KW - dihydrogen evolution

KW - molecular catalysis

KW - nickel(II) complexes

KW - oxygen tolerance

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M3 - RGC 21 - Publication in refereed journal

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SN - 0947-6539

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SP - 8275

EP - 8280

JO - Chemistry - A European Journal

JF - Chemistry - A European Journal

IS - 33

ER -

The Difference Se Makes: A Bio-Inspired Dppf-Supported Nickel Selenolate Complex Boosts Dihydrogen Evolution with High Oxygen Tolerance

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