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    Hydrogen Evolution Catalyzed by Cobaloximes
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    Beckman Institute, California Institute of Technology, Pasadena, California 91125
    * To whom correspondence should be addressed. E-mail addresses: [email protected]; [email protected]; [email protected]
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    Accounts of Chemical Research

    Cite this: Acc. Chem. Res. 2009, 42, 12, 1995–2004
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    https://doi.org/10.1021/ar900253e
    Published November 23, 2009
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    Abstract

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    Natural photosynthesis uses sunlight to drive the conversion of energy-poor molecules (H2O, CO2) to energy-rich ones (O2, (CH2O)n). Scientists are working hard to develop efficient artificial photosynthetic systems toward the “Holy Grail” of solar-driven water splitting. High on the list of challenges is the discovery of molecules that efficiently catalyze the reduction of protons to H2. In this Account, we report on one promising class of molecules: cobalt complexes with diglyoxime ligands (cobaloximes).

    Chemical, electrochemical, and photochemical methods all have been utilized to explore proton reduction catalysis by cobaloxime complexes. Reduction of a CoII-diglyoxime generates a CoI species that reacts with a proton source to produce a CoIII-hydride. Then, in a homolytic pathway, two CoIII-hydrides react in a bimolecular step to eliminate H2. Alternatively, in a heterolytic pathway, protonation of the CoIII-hydride produces H2 and CoIII.

    A thermodynamic analysis of H2 evolution pathways sheds new light on the barriers and driving forces of the elementary reaction steps involved in proton reduction by CoI-diglyoximes. In combination with experimental results, this analysis shows that the barriers to H2 evolution along the heterolytic pathway are, in most cases, substantially greater than those of the homolytic route. In particular, a formidable barrier is associated with CoIII-diglyoxime formation along the heterolytic pathway.

    Our investigations of cobaloxime-catalyzed H2 evolution, coupled with the thermodynamic preference for a homolytic route, suggest that the rate-limiting step is associated with formation of the hydride. An efficient water splitting device may require the tethering of catalysts to an electrode surface in a fashion that does not inhibit association of CoIII-hydrides.

    Copyright © 2009 American Chemical Society

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    Cite this: Acc. Chem. Res. 2009, 42, 12, 1995–2004
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