Electrocatalytic Water Oxidation by a Copper(II) Complex of an Oxidation-Resistant Ligand

Katherine J. Fisher; Kelly L. Materna; Brandon Q. Mercado; Robert H. Crabtree; Gary W. Brudvig

doi:10.1021/acscatal.7b00494

Electrocatalytic Water Oxidation by a Copper(II) Complex of an Oxidation-Resistant Ligand

Katherine J. Fisher, Kelly L. Materna, Brandon Q. Mercado, Robert H. Crabtree, Gary W. Brudvig

Yale University

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

71 Citations (Scopus)

Abstract

The copper(II) complex Cu(pyalk)₂ (pyalk = 2-pyridyl-2-propanoate) is a robust homogeneous water-oxidation electrocatalyst under basic conditions (pH > 10.4). Water oxidation occurs at a relatively low overpotential for copper of 520-580 mV with a turnover frequency of ∼0.7 s^-1. Controlled potential electrolysis experiments over 12 h at 1.1 V vs NHE resulted in the formation of >30 catalytic turnovers of O₂ with only ∼20% catalyst degradation. The robustness of the catalyst under fairly harsh conditions and the low overpotential further highlight the oxidation resistance and strong donor character of pyalk.

Original language	English
Pages (from-to)	3384-3387
Number of pages	4
Journal	ACS Catalysis
Volume	7
Issue number	5
DOIs	https://doi.org/10.1021/acscatal.7b00494
Publication status	Published - May 5 2017

Keywords

OER
copper electrocatalysis
homogeneous electrocatalysis
oxygen-evolution reaction
water-oxidation catalysis

ASJC Scopus subject areas

Catalysis
Chemistry(all)

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10.1021/acscatal.7b00494

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@article{cb3af33527a54b3f8816c24d8c038994,

title = "Electrocatalytic Water Oxidation by a Copper(II) Complex of an Oxidation-Resistant Ligand",

abstract = "The copper(II) complex Cu(pyalk)2 (pyalk = 2-pyridyl-2-propanoate) is a robust homogeneous water-oxidation electrocatalyst under basic conditions (pH > 10.4). Water oxidation occurs at a relatively low overpotential for copper of 520-580 mV with a turnover frequency of ∼0.7 s-1. Controlled potential electrolysis experiments over 12 h at 1.1 V vs NHE resulted in the formation of >30 catalytic turnovers of O2 with only ∼20% catalyst degradation. The robustness of the catalyst under fairly harsh conditions and the low overpotential further highlight the oxidation resistance and strong donor character of pyalk.",

keywords = "OER, copper electrocatalysis, homogeneous electrocatalysis, oxygen-evolution reaction, water-oxidation catalysis",

author = "Fisher, {Katherine J.} and Materna, {Kelly L.} and Mercado, {Brandon Q.} and Crabtree, {Robert H.} and Brudvig, {Gary W.}",

note = "Funding Information: This work was supported the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences as part of the Argonne-Northwestern Solar Energy Research (ANSER) Energy Frontier Research Center under Award Number DESC0001059. K.J.F acknowledges the National Science Foundation Graduate Research Fellowship Program (Grant No. DGE1122492). We also thank the funding provided by a generous donation from the TomKat Charitable Trust.",

year = "2017",

month = may,

day = "5",

doi = "10.1021/acscatal.7b00494",

language = "English",

volume = "7",

pages = "3384--3387",

journal = "ACS Catalysis",

issn = "2155-5435",

publisher = "American Chemical Society",

number = "5",

}

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T1 - Electrocatalytic Water Oxidation by a Copper(II) Complex of an Oxidation-Resistant Ligand

AU - Fisher, Katherine J.

AU - Materna, Kelly L.

AU - Mercado, Brandon Q.

AU - Crabtree, Robert H.

AU - Brudvig, Gary W.

N1 - Funding Information: This work was supported the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences as part of the Argonne-Northwestern Solar Energy Research (ANSER) Energy Frontier Research Center under Award Number DESC0001059. K.J.F acknowledges the National Science Foundation Graduate Research Fellowship Program (Grant No. DGE1122492). We also thank the funding provided by a generous donation from the TomKat Charitable Trust.

PY - 2017/5/5

Y1 - 2017/5/5

N2 - The copper(II) complex Cu(pyalk)2 (pyalk = 2-pyridyl-2-propanoate) is a robust homogeneous water-oxidation electrocatalyst under basic conditions (pH > 10.4). Water oxidation occurs at a relatively low overpotential for copper of 520-580 mV with a turnover frequency of ∼0.7 s-1. Controlled potential electrolysis experiments over 12 h at 1.1 V vs NHE resulted in the formation of >30 catalytic turnovers of O2 with only ∼20% catalyst degradation. The robustness of the catalyst under fairly harsh conditions and the low overpotential further highlight the oxidation resistance and strong donor character of pyalk.

AB - The copper(II) complex Cu(pyalk)2 (pyalk = 2-pyridyl-2-propanoate) is a robust homogeneous water-oxidation electrocatalyst under basic conditions (pH > 10.4). Water oxidation occurs at a relatively low overpotential for copper of 520-580 mV with a turnover frequency of ∼0.7 s-1. Controlled potential electrolysis experiments over 12 h at 1.1 V vs NHE resulted in the formation of >30 catalytic turnovers of O2 with only ∼20% catalyst degradation. The robustness of the catalyst under fairly harsh conditions and the low overpotential further highlight the oxidation resistance and strong donor character of pyalk.

KW - OER

KW - copper electrocatalysis

KW - homogeneous electrocatalysis

KW - oxygen-evolution reaction

KW - water-oxidation catalysis

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