半夹心钌分子催化剂的水氧化电催化

设计和合成以五甲基环戊二烯基(Cp^*)半夹心钌配合物为代表的一种具有开放的空间结构和高电荷密度的分子催化剂,通过对配体的调控,成功筛选出具有良好水氧化电催化活性、易固载到电极表面且在强碱性环境下抗水解的［Cp^*Ru(PPh₃)₂Cl］Cl配合物分子.电化学和在线微分电化学质谱实验表明:该分子可提供易于被进攻Ru(Ⅴ)活性中心,显著加速水氧化生成O₂的反应速率.

Half-Sandwich Ruthenium Molecular Catalyst Towards Water Oxidation Electrolysis

A half-sandwich ruthenium complex for the water oxidation reaction electrolysis with one pentamethylcyclopentadienyl(Cp^*)ligand was designed and prepared, which is featured with an open geometric configuration and a high density of charge. By tuning the other ligands, a ［Cp^*Ru(PPh₃)₂Cl］Cl molecule was screened successfully which encompassed a superior catalytic activity, a facile fixation to the electrode, and a high resistance to the hydrolysis reaction under the strong-alkaline condition. Combining the electrochemical and on-line differential electrochemical mass spectrometry studies, it is proposed that this molecular Ru catalyst can provide accessible Ru(Ⅴ)active center which can remarkably accelerate the water oxidation to O₂.