Literature DB >> 22786932

Catalytic hydrogen evolution from a covalently linked dicobaloxime.

Carolyn N Valdez1, Jillian L Dempsey, Bruce S Brunschwig, Jay R Winkler, Harry B Gray.   

Abstract

A dicobaloxime in which monomeric Co(III) units are linked by an octamethylene bis(glyoxime) catalyzes the reduction of protons from p-toluenesulfonic acid as evidenced by electrocatalytic waves at -0.4 V vs. the saturated calomel electrode (SCE) in acetonitrile solutions. Rates of hydrogen evolution were determined from catalytic current peak heights (k(app) = 1100 ± 70 M(-1) s(-1)). Electrochemical experiments reveal no significant enhancement in the rate of H(2) evolution from that of a monomeric analogue: The experimental rate law is first order in catalyst and acid consistent with previous findings for similar mononuclear cobaloximes. Our work suggests that H(2) evolution likely occurs by protonation of reductively generated Co(II)H rather than homolysis of two Co(III)H units.

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Year:  2012        PMID： 22786932      PMCID： PMC3465440          DOI： 10.1073/pnas.1118329109

Source DB:  PubMed          Journal:  Proc Natl Acad Sci U S A        ISSN： 0027-8424            Impact factor:   11.205


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