A nickel phosphine complex as a fast and efficient hydrogen production catalyst

Lu Gan; Thomas L. Groy; Tarakeshwar Pilarisetty; Shobeir K S Mazinani; Jason Shearer; Vladimiro Mujica; Anne Jones

doi:10.1021/ja509779q

A nickel phosphine complex as a fast and efficient hydrogen production catalyst

Lu Gan, Thomas L. Groy, Tarakeshwar Pilarisetty, Shobeir K S Mazinani, Jason Shearer, Vladimiro Mujica, Anne Jones

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130 Scopus citations

Abstract

(Chemical Equation Presented) Here we report the electrocatalytic reduction of protons to hydrogen by a novel S₂P₂ coordinated nickel complex, [Ni(bdt)(dppf)] (bdt = 1,2-benzenedithiolate, dppf = 1,1′-bis(diphenylphosphino)ferrocene). The catalysis is fast and effi cient with a turnover frequency of 1240 s^-1 and an overpotential of only 265 mV for half activity at low acid concentrations. Furthermore, catalysis is possible using a weak acid, and the complex is stable for at least 4 h in acidic solution. Calculations of the system carried out at the density functional level of theory (DFT) are consistent with a mechanism for catalysis in which both protonations take place at the nickel center.

Original language	English (US)
Pages (from-to)	1109-1115
Number of pages	7
Journal	Journal of the American Chemical Society
Volume	137
Issue number	3
DOIs	https://doi.org/10.1021/ja509779q
State	Published - Jan 28 2015

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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10.1021/ja509779q

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title = "A nickel phosphine complex as a fast and efficient hydrogen production catalyst",

abstract = "(Chemical Equation Presented) Here we report the electrocatalytic reduction of protons to hydrogen by a novel S2P2 coordinated nickel complex, [Ni(bdt)(dppf)] (bdt = 1,2-benzenedithiolate, dppf = 1,1′-bis(diphenylphosphino)ferrocene). The catalysis is fast and effi cient with a turnover frequency of 1240 s-1 and an overpotential of only 265 mV for half activity at low acid concentrations. Furthermore, catalysis is possible using a weak acid, and the complex is stable for at least 4 h in acidic solution. Calculations of the system carried out at the density functional level of theory (DFT) are consistent with a mechanism for catalysis in which both protonations take place at the nickel center.",

author = "Lu Gan and Groy, {Thomas L.} and Tarakeshwar Pilarisetty and Mazinani, {Shobeir K S} and Jason Shearer and Vladimiro Mujica and Anne Jones",

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T1 - A nickel phosphine complex as a fast and efficient hydrogen production catalyst

AU - Gan, Lu

AU - Groy, Thomas L.

AU - Pilarisetty, Tarakeshwar

AU - Mazinani, Shobeir K S

AU - Shearer, Jason

AU - Mujica, Vladimiro

AU - Jones, Anne

PY - 2015/1/28

Y1 - 2015/1/28

N2 - (Chemical Equation Presented) Here we report the electrocatalytic reduction of protons to hydrogen by a novel S2P2 coordinated nickel complex, [Ni(bdt)(dppf)] (bdt = 1,2-benzenedithiolate, dppf = 1,1′-bis(diphenylphosphino)ferrocene). The catalysis is fast and effi cient with a turnover frequency of 1240 s-1 and an overpotential of only 265 mV for half activity at low acid concentrations. Furthermore, catalysis is possible using a weak acid, and the complex is stable for at least 4 h in acidic solution. Calculations of the system carried out at the density functional level of theory (DFT) are consistent with a mechanism for catalysis in which both protonations take place at the nickel center.

AB - (Chemical Equation Presented) Here we report the electrocatalytic reduction of protons to hydrogen by a novel S2P2 coordinated nickel complex, [Ni(bdt)(dppf)] (bdt = 1,2-benzenedithiolate, dppf = 1,1′-bis(diphenylphosphino)ferrocene). The catalysis is fast and effi cient with a turnover frequency of 1240 s-1 and an overpotential of only 265 mV for half activity at low acid concentrations. Furthermore, catalysis is possible using a weak acid, and the complex is stable for at least 4 h in acidic solution. Calculations of the system carried out at the density functional level of theory (DFT) are consistent with a mechanism for catalysis in which both protonations take place at the nickel center.

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A nickel phosphine complex as a fast and efficient hydrogen production catalyst

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CCDC 941160: Experimental Crystal Structure Determination

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A nickel phosphine complex as a fast and efficient hydrogen production catalyst

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CCDC 941160: Experimental Crystal Structure Determination

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