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

Research output: Contribution to journal › Article › peer-review

98 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
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

Access to Document

10.1021/ja509779q

Fingerprint Dive into the research topics of 'A nickel phosphine complex as a fast and efficient hydrogen production catalyst'. Together they form a unique fingerprint.

Cite this

@article{ca5bfe6c3f38465caaf68a84e7f3f757,

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",

year = "2015",

month = jan,

day = "28",

doi = "10.1021/ja509779q",

language = "English (US)",

volume = "137",

pages = "1109--1115",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "3",

}

TY - JOUR

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.

UR - http://www.scopus.com/inward/record.url?scp=84921845393&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84921845393&partnerID=8YFLogxK

U2 - 10.1021/ja509779q

DO - 10.1021/ja509779q

M3 - Article

C2 - 25562523

AN - SCOPUS:84921845393

VL - 137

SP - 1109

EP - 1115

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 3

ER -