期刊
SUPRAMOLECULAR CHEMISTRY
卷 23, 期 3-4, 页码 287-296出版社
TAYLOR & FRANCIS LTD
DOI: 10.1080/10610278.2010.527976
关键词
water splitting; coordination polymers; metal organic frameworks
资金
- Ministry of Education, Culture, Sports, Science and Technology of Japan [19350077]
In this study we investigated the photochemical production of hydrogen from water using three heterogeneous microporous ruthenium coordination polymers [Ru2(p-BDC)2X]n (p-BDC=1,4-benzenedicarboxylate, X=Cl, Br and BF4) in the presence of multi-component systems. The order of catalytic performances is [Ru2(p-BDC)2Br]n[Ru2(p-BDC)2BF4]n[Ru2(p-BDC)2Cl]n. The most active catalyst, [Ru2(p-BDC)2Br]n, caused the evolution of 46.7mol hydrogen molecules with a turn-over number of 18.7 based on [Ru2(p-BDC)2Br]n under visible light irradiation for 4h. We ascertained that the differences in catalytic activities originated from (1) the efficiency of the quenching of methyl-viologen radicals by [Ru2(p-BDC)2X]n and (2) the durability of the structure in the reaction. In order to examine the catalytic reaction mechanism, we performed theoretical calculations for neutral model structures [Ru2(HCOO)4X(H2O)] (X=Cl, Br), one-electron reduction model complexes [Ru2(HCOO)4X(H2O)]- and deduced intermediate model structures [H-Ru2(HCOO)4X] using broken-symmetry hybrid density functional theory methods.
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