Catalytic Water Oxidation by a Bio-inspired Nickel Complex with a Redox-Active Ligand

Dong Wang; Charlie O. Bruner

doi:10.1021/acs.inorgchem.7b02166

Catalytic Water Oxidation by a Bio-inspired Nickel Complex with a Redox-Active Ligand

Dong Wang
, Charlie O. Bruner

Chemistry and Biochemistry

University of Montana

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

82 Scopus citations

Abstract

The oxidation of water (H₂O) to dioxygen (O₂) is important in natural photosynthesis. One of nature's strategies for managing such multi-electron transfer reactions is to employ redox-active metal-organic cofactor arrays. One prototype example is the copper tyrosinate active site found in galactose oxidase. In this work, we have implemented such a strategy to develop a bio-inspired nickel phenolate complex capable of catalyzing the oxidation of H₂O to O₂ electrochemically at neutral pH with a modest overpotential. Employment of the redox-active ligand turned out to be a useful strategy to avoid the formation of high-valent nickel intermediates while a reasonable turnover rate (0.15 s^-1) is retained.

Original language	English
Pages (from-to)	13638-13641
Number of pages	4
Journal	Inorganic Chemistry
Volume	56
Issue number	22
DOIs	https://doi.org/10.1021/acs.inorgchem.7b02166
State	Published - Nov 20 2017

Funding

Support of this work was provided by the Center for Biomolecular Structure and Dynamics CoBRE (Grant NIGMS P20GM103546) and the University of Montana. C.O.B. thanks the M. J. Murdock Charitable Trust for a Partnership in Science award (2015409: JAT: 2/25/2016). We thank Daniel A. Decato for his assistance in solving the crystal structures.

Funders	Funder number
Center for Biomolecular Structure and Dynamics
P20GM103546

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title = "Catalytic Water Oxidation by a Bio-inspired Nickel Complex with a Redox-Active Ligand",

abstract = "The oxidation of water (H2O) to dioxygen (O2) is important in natural photosynthesis. One of nature's strategies for managing such multi-electron transfer reactions is to employ redox-active metal-organic cofactor arrays. One prototype example is the copper tyrosinate active site found in galactose oxidase. In this work, we have implemented such a strategy to develop a bio-inspired nickel phenolate complex capable of catalyzing the oxidation of H2O to O2 electrochemically at neutral pH with a modest overpotential. Employment of the redox-active ligand turned out to be a useful strategy to avoid the formation of high-valent nickel intermediates while a reasonable turnover rate (0.15 s-1) is retained.",

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N2 - The oxidation of water (H2O) to dioxygen (O2) is important in natural photosynthesis. One of nature's strategies for managing such multi-electron transfer reactions is to employ redox-active metal-organic cofactor arrays. One prototype example is the copper tyrosinate active site found in galactose oxidase. In this work, we have implemented such a strategy to develop a bio-inspired nickel phenolate complex capable of catalyzing the oxidation of H2O to O2 electrochemically at neutral pH with a modest overpotential. Employment of the redox-active ligand turned out to be a useful strategy to avoid the formation of high-valent nickel intermediates while a reasonable turnover rate (0.15 s-1) is retained.

AB - The oxidation of water (H2O) to dioxygen (O2) is important in natural photosynthesis. One of nature's strategies for managing such multi-electron transfer reactions is to employ redox-active metal-organic cofactor arrays. One prototype example is the copper tyrosinate active site found in galactose oxidase. In this work, we have implemented such a strategy to develop a bio-inspired nickel phenolate complex capable of catalyzing the oxidation of H2O to O2 electrochemically at neutral pH with a modest overpotential. Employment of the redox-active ligand turned out to be a useful strategy to avoid the formation of high-valent nickel intermediates while a reasonable turnover rate (0.15 s-1) is retained.

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JO - Inorganic Chemistry

JF - Inorganic Chemistry

IS - 22

ER -

Catalytic Water Oxidation by a Bio-inspired Nickel Complex with a Redox-Active Ligand

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