期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 135, 期 45, 页码 16997-17003出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja407176p
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资金
- Swedish Research Council
- Swedish Energy Agency
- Knut & Alice Wallenberg Foundation
- Austrian Science Fund (FWF)
- Erwin-Schrodinger fellowship [J 3193-N17]
- National Science Foundation, Division of Materials Research [DMR-1262226]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1262226] Funding Source: National Science Foundation
A molecular proton reduction catalyst [FeFe](dcbdt)(CO)(6) (1, dcbdt = 1,4-dicarboxylbenzene-2,3-dithiolate) with structural similarities to [FeFe]-hydrogenase active sites has been incorporated into a highly robust Zr(IV)-based metal-organic framework (MOF) by postsynthetic exchange (PSE). The PSE protocol is crucial as direct solvothermal synthesis fails to produce the functionalized MOF. The molecular integrity of the organometallic site within the MOF is demonstrated by a variety of techniques, including X-ray absorption spectroscopy. In conjunction with [Ru(bpy)(3)](2+) as a photosensitizer and ascorbate as an electron donor, MOF-[FeFe](dcbdt)(CO)(6) catalyzes photochemical hydrogen evolution in water at pH 5. The immobilized catalyst shows substantially improved initial rates and overall hydrogen production when compared to a reference system of complex 1 in solution. Improved catalytic performance is ascribed to structural stabilization of the complex when incorporated in the MOF as well as the protection of reduced catalysts 1(-) and 1(2-) from undesirable charge recombination with oxidized ascorbate.
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