期刊
DALTON TRANSACTIONS
卷 39, 期 12, 页码 3050-3056出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/b921067a
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资金
- National Science Foundation [CHE0527003, CHE-0741837]
- Direct For Mathematical & Physical Scien [0749530] Funding Source: National Science Foundation
- Division Of Chemistry [0741837] Funding Source: National Science Foundation
The [FeFe] hydrogenase enzyme active site inspired complexes [Fe(2)(mu-C(6)H(4)S(2))(CO)(5)PTA] (1PTA) and [Fe(2)(mu-C(6)H(4)S(2))(CO)(4)PTA(2)] (1PTA(2)) (PTA = 1,3,5-triaza-7-phosphaadamantane) were synthesized and characterized. The ability of 1PTA and 1PTA(2) to catalytically produce molecular hydrogen in solution from the weak acid acetic acid was examined electrochemically and compared to previous studies on the all carbonyl containing analogue [Fe(2)(mu-C(6)H(4)S(2))(CO)(6)] (1). Computational methods and cyclic voltammograms indicated that the substitution of CO ligands by PTA in 1 resulted in markedly different reduction chemistry. Both 1PTA and 1PTA(2) catalytically produce molecular hydrogen from acetic acid, however, the mechanism by which 1 and 1PTA and 1PTA(2) catalyze hydrogen differ in the initial reductive processes.
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