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Edited by Thomas J. Meyer, University of North Carolina at Chapel Hill, Chapel Hill, NC, and approved June 14, 2012 (received for review February 7, 2012)
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 (kapp = 1100 ± 70 M-1 s-1). Electrochemical experiments reveal no significant enhancement in the rate of H2 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 H2 evolution likely occurs by protonation of reductively generated CoIIH rather than homolysis of two CoIIIH units.
Footnotes
- ↵1To whom correspondence may be addressed. E-mail: bsb{at}caltech.edu or winklerj{at}caltech.edu or hbgray{at}caltech.edu.
Author contributions: C.N.V., J.L.D., J.R.W., and H.B.G. designed research; C.N.V. and J.L.D. performed research; C.N.V. and J.L.D. contributed new reagents/analytic tools; C.N.V., J.L.D., and B.S.B. analyzed data; and C.N.V., J.L.D., J.R.W., and H.B.G. wrote the paper.
The authors declare no conflict of interest.
This article is a PNAS Direct Submission.
This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.1073/pnas.1118329109/-/DCSupplemental.
Catalytic hydrogen evolution
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