2011
DOI: 10.1021/ja207842r
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A Cobalt–Dithiolene Complex for the Photocatalytic and Electrocatalytic Reduction of Protons

Abstract: The complex [Co(bdt)(2)](-) (where bdt = 1,2-benzenedithiolate) is an active catalyst for the visible light driven reduction of protons from water when employed with Ru(bpy)(3)(2+) as the photosensitizer and ascorbic acid as the sacrificial electron donor. At pH 4.0, the system exhibits very high activity, achieving >2700 turnovers with respect to catalyst and an initial turnover rate of 880 mol H(2)/mol catalyst/h. The same complex is also an active electrocatalyst for proton reduction in 1:1 CH(3)CN/H(2)O in… Show more

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Cited by 374 publications
(328 citation statements)
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“…The CoðmntÞ − 2 catalyst 4 achieves the highest activity of the dithiolene complexes, achieving a total TON of approximately 9,000 (measured with respect to cobalt), with an initial turnover frequency up to 3450 h −1 . This level of activity places 4 among the most active H 2 generating catalysts reported (26,30,31). The systems remain active for 6-10 h before decomposition of catalyst and chromophore contribute to a gradual decrease in hydrogen evolution.…”
mentioning
confidence: 81%
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“…The CoðmntÞ − 2 catalyst 4 achieves the highest activity of the dithiolene complexes, achieving a total TON of approximately 9,000 (measured with respect to cobalt), with an initial turnover frequency up to 3450 h −1 . This level of activity places 4 among the most active H 2 generating catalysts reported (26,30,31). The systems remain active for 6-10 h before decomposition of catalyst and chromophore contribute to a gradual decrease in hydrogen evolution.…”
mentioning
confidence: 81%
“…1,2-Benzenedithiol, 3,6-dichlorobenzenedithiol, sodium maleonitriledithiolate, toluenedithiol, cobalt(II) tetrafluoroborate hexahydrate, ½RuðbpyÞ 3 Cl 2 , potassium tert-butoxide, and tetrabutylammonium bromide were purchased from Aldrich and used without further purification. Catalyst 1 was synthesized according to a literature procedure (30).…”
Section: Methodsmentioning
confidence: 99%
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“…Dithiolenes are well-known to exhibit noninnocent redox behavior, affording ligand-centered reductions and oxidations. 11,12,143,153,161 This ligand non-innocence offers extremely reactive thiyl radicals. As detailed in ( Figure 9A) the facial arrangement of the PS chelates in [ReL 3 ] n enforces a symmetry preferred interligand addition route.…”
Section: Culmentioning
confidence: 99%