To mimic [FeFe] hydrogenases (H2ases) in nature, molecular photocatalysts , , and anchoring rhenium(I) complex S to one of the iron cores of [FeFe]-H2ases model complex C, have been constructed for H2 generation by visible light in homogeneous solution. The time-dependence of H2 evolution and a spectroscopic study demonstrate that the orientation of S and the specific bridge in , , and are important both for the electron-transfer step from the excited S* to the catalytic C, and the formation of unprecedented long-lived charge separation for (780 μs), , and (>2 ms) in [FeFe]-H2ases mimics. The fast forward electron-transfer step from the excited S* to the catalytic C but the slow back electron-transfer step of the charge-recombination in the designed photocatalysts , , and are reminiscent of the behavior of [FeFe]-H2ases in nature.
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