Reduction of oxygen catalyzed by nickel diphosphine complexes with positioned pendant amines

Jenny Y. Yang; R. Morris Bullock; William G. Dougherty; W. Scott Kassel; Brendan Twamley; Daniel L. DuBois; M. Rakowski DuBois

doi:10.1039/B921245K

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Dalton Transactions

Issue 12, 2010

The international journal for inorganic, organometallic and bioinorganic chemistry

Impact Factor 3.838 48 Issues per Year Indexed in MEDLINE

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Reduction of oxygen catalyzed by nickel diphosphine complexes with positioned pendant amines

Jenny Y. Yang,^a R. Morris Bullock,^a William G. Dougherty,^b W. Scott Kassel,^b Brendan Twamley,^c Daniel L. DuBois*^a and M. Rakowski DuBois*^a

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Chemical and Materials Sciences Division, Pacific Northwest National Laboratory, Richland, USA
E-mail: mary.rakowskidubois@pnl.gov

Department of Chemistry, Villanova University, Villanova, USA

Department of Chemistry, University of Idaho, Moscow, USA

Dalton Trans., 2010,39, 3001-3010

DOI: 10.1039/B921245K
Received 12 Oct 2009, Accepted 30 Nov 2009
First published online 19 Jan 2010

This article is part of themed collection: Bioinspired catalysis

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Abstract
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Nickel(II) bis(diphosphine) complexes that contain positioned bases in the second coordination sphere have been found to catalyze the reduction of O₂ with H₂ to selectively form water. The complexes also serve as electrocatalysts for the reduction of O₂ with the addition of a weak acid. In contrast, a closely related nickel diphosphine complex without the positioned bases is catalytically inactive for O₂ reduction. These results indicate that pendant bases in synthetic catalysts for O₂ reduction can play a similar role to proton relays in enzymes, and that such relays should be considered in the design of catalysts for multi-electron and multi-proton reactions.

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Jenny Y. Yang
R. Morris Bullock
William G. Dougherty
W. Scott Kassel
Brendan Twamley
Daniel L. DuBois
M. Rakowski DuBois

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