Redox tuning in Pt(bpy)-viologen catalyst-acceptor dyads enabling photocatalytic hydrogen evolution from water
Redox tuning in Pt(bpy)-viologen catalyst-acceptor dyads enabling photocatalytic hydrogen evolution from water
复制标题
Pt(bpy)-紫罗碱催化剂-受体二元组中的氧化还原调节使得光催化从水中析氢成为可能
DOI：
10.1039/d1cc00903f
复制
发表时间：
2021
影响因子：
4.9
通讯作者：
Sakai Ken
中科院分区：
文献类型：
--
作者：
Yatsuzuka Koichi;Yamauchi Kosei;Sakai Ken
一个基于Pt（II）的光-析氢分子器件拴到二甲基取代的紫精（Pt（bpy）（dmMV 2+）2），提供更高的驱动力的析氢反应（HER）比非甲基化的类似物（Pt（bpy）（MV 2+）2），被发现表现出改善的光催化性能。所观察到的行为被解释为多个HER途径所采取的演变H2的双重和三重减少通过连续的光驱动步骤产生的物种。虽然活性仍然被杀死的德克斯特型能量转移淬火，我们的研究结果提供了新的设计策略，更精细的调整控制光催化HER分子器件的发展。
A Pt(II)-based photo-hydrogen-evolving molecular device tethered to dimethyl-substituted viologens (Pt(bpy)(dmMV2+)2), providing higher driving force for hydrogen evolution reaction (HER) than the non-methylated analogue (Pt(bpy)(MV2+)2), is found to exhibit improved photocatalytic performance. The observed behaviors are explained by the multiple HER pathways taken by evolving H2 by the doubly and triply reduced species generated via consecutive photo-driven steps. Although the activity is still killed by the Dexter-type energy transfer quenching, our results provide new design strategies towards the development of more finely tuned molecular devices controlling the photocatalytic HER.