Molecular cobalt pentapyridine catalysts for generating hydrogen from water

Yujie Sun; Julian P. Bigi; Nicholas A. Piro; Ming Lee Tang; Jeffrey R. Long; Christopher J. Chang

doi:10.1021/ja202743r

Molecular cobalt pentapyridine catalysts for generating hydrogen from water

Yujie Sun, Julian P. Bigi, Nicholas A. Piro, Ming Lee Tang, Jeffrey R. Long, Christopher J. Chang

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

406 Scopus citations

Abstract

A set of robust molecular cobalt catalysts for the generation of hydrogen from water is reported. The cobalt complex supported by the parent pentadentate polypyridyl ligand PY5Me₂ features high stability and activity and 100% Faradaic efficiency for the electrocatalytic production of hydrogen from neutral water, with a turnover number reaching 5.5 × 10⁴ mol of H₂ per mole of catalyst with no loss in activity over 60 h. Control experiments establish that simple Co(II) salts, the free PY5Me₂ ligand, and an isostructural PY5Me₂ complex containing redox-inactive Zn(II) are all ineffective for this reaction. Further experiments demonstrate that the overpotential for H₂ evolution can be tuned by systematic substitutions on the ancillary PY5Me₂ scaffold, presaging opportunities to further optimize this first-generation platform by molecular design.

Original language	English (US)
Pages (from-to)	9212-9215
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	133
Issue number	24
DOIs	https://doi.org/10.1021/ja202743r
State	Published - Jun 22 2011
Externally published	Yes

All Science Journal Classification (ASJC) codes

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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title = "Molecular cobalt pentapyridine catalysts for generating hydrogen from water",

abstract = "A set of robust molecular cobalt catalysts for the generation of hydrogen from water is reported. The cobalt complex supported by the parent pentadentate polypyridyl ligand PY5Me2 features high stability and activity and 100% Faradaic efficiency for the electrocatalytic production of hydrogen from neutral water, with a turnover number reaching 5.5 × 104 mol of H2 per mole of catalyst with no loss in activity over 60 h. Control experiments establish that simple Co(II) salts, the free PY5Me2 ligand, and an isostructural PY5Me2 complex containing redox-inactive Zn(II) are all ineffective for this reaction. Further experiments demonstrate that the overpotential for H2 evolution can be tuned by systematic substitutions on the ancillary PY5Me2 scaffold, presaging opportunities to further optimize this first-generation platform by molecular design.",

author = "Yujie Sun and Bigi, {Julian P.} and Piro, {Nicholas A.} and Tang, {Ming Lee} and Long, {Jeffrey R.} and Chang, {Christopher J.}",

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T1 - Molecular cobalt pentapyridine catalysts for generating hydrogen from water

AU - Sun, Yujie

AU - Bigi, Julian P.

AU - Piro, Nicholas A.

AU - Tang, Ming Lee

AU - Long, Jeffrey R.

AU - Chang, Christopher J.

PY - 2011/6/22

Y1 - 2011/6/22

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AB - A set of robust molecular cobalt catalysts for the generation of hydrogen from water is reported. The cobalt complex supported by the parent pentadentate polypyridyl ligand PY5Me2 features high stability and activity and 100% Faradaic efficiency for the electrocatalytic production of hydrogen from neutral water, with a turnover number reaching 5.5 × 104 mol of H2 per mole of catalyst with no loss in activity over 60 h. Control experiments establish that simple Co(II) salts, the free PY5Me2 ligand, and an isostructural PY5Me2 complex containing redox-inactive Zn(II) are all ineffective for this reaction. Further experiments demonstrate that the overpotential for H2 evolution can be tuned by systematic substitutions on the ancillary PY5Me2 scaffold, presaging opportunities to further optimize this first-generation platform by molecular design.

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Molecular cobalt pentapyridine catalysts for generating hydrogen from water

Abstract

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