Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 133, Issue 45, Pages 18070-18073Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja2078015
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Funding
- NSF Center for Chemical Innovation on Solar Fuels (CCI Solar) [CHE-0802907, CHE-0947829]
- Stanford Global Climate and Energy Project (GCEP)
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0802907] Funding Source: National Science Foundation
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A cobalt bis(iminopyridine) complex is a highly active electrocatalyst for water reduction, with an estimated apparent second order rate constant k(app) <= 10(7) M-1 s(-1) over a range of buffer/salt concentrations. Scan rate dependence data are consistent with freely diffusing electro-active species over pH 4-9 at room temperature for each of two catalytic reduction events, one of which is believed to be ligand based. Faradaic H-2 yields up to 87 +/- 10% measured in constant potential electrolyses (-1.4 V vs SCE) confirm high reactivity and high fidelity in a catalyst supported by the noninnocent bis(iminopyridine) ligand. A mechanism involving initial reduction of Co2+ and subsequent protonation is proposed.
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