Molecular catalysts for oxidation of hydrogen and production of hydrogen: Shoving protons around with pendant amines

R. Morris Bullock, Jenny Y. Yang, Eric S. Wiedner, Kevin D. Welch, Daniel L. Dubois

Research output: Contribution to journalConference article

Abstract

Catalysts that efficiently convert electrical energy into chemical bonds in fuels, or the reverse, converting chemical energy to electrical energy, will play a vital role in a flexible and sustainable energy supply in the future. Incorporation of pendant amines into diphosphine ligands can lead to fast catalytic rates and low overpotentials in electrocatalytic reactions. The fastest rates for oxidation and production of hydrogen are obtained for nickel catalysts with two positioned proton relays. In contrast, cobalt complexes such as [Co(P2N2)(NCMe)3]2+, with just one P2N2 ligand, catalyze the production of hydrogen. Binding and heterolytic cleavage of dihydrogen is also observed for complexes of manganese with pendant amines on the diphosphine. In all of these reactions, pendant amines in the second coordination sphere influence the reactivity by accelerating proton movement between the metal center and solution, and by facilitating the binding and heterolytic cleavage of hydrogen.

Original languageEnglish
JournalACS National Meeting Book of Abstracts
Publication statusPublished - Dec 1 2010
Event240th ACS National Meeting and Exposition - Boston, MA, United States
Duration: Aug 22 2010Aug 26 2010

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

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