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[Fe2S2-Ag]-Hydrogenase Active-Site-Containing Coordination Polymers and Their Photocatalytic H2 Evolution Reaction
Xinhui Chen1, Fan Yang1, Congcong Han1
1College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Key Laboratory of Molecular and Nano Probes, Ministry of Education, Shandong Normal University, Jinan 250014, P. R. China.
Abstract:
Three [Fe2S2-Ag]-hydrogenase active-site-containing coordination polymers (CPs), {[Fe2S2-Ag1](4-cpmt)2(CO)6(ClO4-)} (1), {[Fe2S2-Ag2](4-cpmt)2(CO)6(OTf-)2(benzene)} (2), and {[Fe2S2-Ag2](3-cpmt)2(CO)6(ClO4-)2} (3), were obtained by a direct synthesis method from ligands [FeFe](4-cpmt)2(CO)6 [L1; 4-cpmt = (4-cyanophenyl)methanethiolate] and [FeFe](3-cpmt)2(CO)6 [L2; 3-cpmt = (3-cyanophenyl)methanethiolate] with silver salts. 1-3 represent the first examples of [FeFe]-hydrogenase-based CPs. It was worth noting that the Ag-S bonding between the Ag centers and S atoms of a [Fe2S2] cluster produced a novel [Fe2S2-Ag] (x = 1 or 2) catalytic site in all three polymers. The results of photochemical H2 generation experiments indicated that 2 and 3 containing [Fe2S2-Ag2] active sites showed obviously improved catalytic performances compared with ligands L1 and L2 and [Fe2S2-Ag1]-containing 1. This work provides a pioneering strategy for the direct synthesis of [Fe2S2]-based CPs or metal-organic frameworks.
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