HOMOGENEOUS WATER OXIDATION CATALYZED BY CO-BASED POLYOXOMETALATES

Yurii Geletii 1 James Vickers 1 Hongjin Lv 1 Petro Zhuk 2 Guibo Zhu 1 Zhen Luo 1 Jie Song 1 Yong Din 1 John Fielden 1 Chongchao Zhao 1 John Bacsa 1 Djamaladdin Musaev 3 Craig Hill 1
1Department of Chemistry, Emory University, Atlanta
2Department of Applied Mathematics, National Aviation University, Kiev
3Cherry L. Emerson Center for Scientific Computation, Emory University, Atlanta

Catalytic water oxidation is the crucial challenge in the conversion of sunlight energy into such green fuels as hydrogen from water: H2O + sunlight ® H2 + ½ O2. At present, the water oxidation catalysts (WOCs), based on abundant metals such as cobalt, are the most efficient and promising for further development. We have developed a family of Co-containing molecular WOCs containing different oxidatively robust polydentate polyoxometalate ligands with different hydrolytic stabilities and catalytic activities. Two representatives of this class of WOCs are the polyoxometalates (POMs) of formula [Co4(H2O)2(XW9O34)2]10-, X = PIV (1-P2) or VV (1-V2). While, they are isostructural with two of the Co(II) centres accessible to water, their activities and stabilities are very different. At present, the homogeneous molecular 1-V2 catalyst is by far the fastest WOC to date. New experimental data on stability of Co-based polyoxometalates will be reported. Kinetic models of catalytic water oxidation will be also discussed.









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