【摘 要】
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Water oxidation plays a critical role in solar water splitting.[1] Herein we report the crystallographic characterization of a RuⅢ-O-RuⅣ-O-RuⅢ type trinuclear ruthenium intermediate to shed light on t
【机 构】
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State Key Laboratory of Fine Chemicals,Dalian University of Technology,Dalian 116024,China
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Water oxidation plays a critical role in solar water splitting.[1] Herein we report the crystallographic characterization of a RuⅢ-O-RuⅣ-O-RuⅢ type trinuclear ruthenium intermediate to shed light on the mechanistic details of photocatalytic water oxidation by a mononuclear catalyst Ru(bda)(pic)2(H2bda = 2,2′-bipyridine-6,6′-dicarboxylic acid; pic = 4-picoline)in neutral aqueous solution.[2-4] The formation of ruthenium trimer by comproportionation of RuⅡ and RuⅣ=O was fully identified in chemical,electrochemical and photochemical water oxidation,respectively.Under neutral conditions,the ruthenium trimer was found to re-enter the catalytic cycle by oxidative decompose to ruthenium monomer accompanied with the generation of inactive species,which competes with the catalytic pathway of oxygen evolution.
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