A synthetic nickel electrocatalyst with a turnover frequency above 100,000 s-1 for H2 production

Monte L. Helm, Michael P. Stewart, R. Morris Bullock, M. Rakowski DuBois, Daniel L. DuBois

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761 Citations (Scopus)

Abstract

Reduction of acids to molecular hydrogen as a means of storing energy is catalyzed by platinum, but its low abundance and high cost are problematic. Precisely controlled delivery of protons is critical in hydrogenase enzymes in nature that catalyze hydrogen (H2) production using earth-abundant metals (iron and nickel). Here, we report that a synthetic nickel complex, [Ni(PPh2NPh)2](BF4)2, (PPh2NPh = 1,3,6-triphenyl-1-aza-3,6- diphosphacycloheptane), catalyzes the production of H2 using protonated dimethylformamide as the proton source, with turnover frequencies of 33,000 per second (s-1) in dry acetonitrile and 106,000 s-1 in the presence of 1.2 M of water, at a potential of -1.13 volt (versus the ferrocenium/ferrocene couple). The mechanistic implications of these remarkably fast catalysts point to a key role of pendant amines that function as proton relays.

Original languageEnglish
Pages (from-to)863-866
Number of pages4
JournalScience
Volume333
Issue number6044
DOIs
Publication statusPublished - Aug 12 2011

ASJC Scopus subject areas

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