Abstract
Directional electron flow in the photocatalyst enables efficient charge separation, which is essential for efficient photocatalysis of H2 production. Here, we report a novel class of tetracationic cyclophanes (7) incorporating bipyridine Pt(II) and selenoviologen. X‐ray single‐crystal structures reveal that 7 not only fixes the distances and spatial positions between its individual units but also exhibits a box‐like rigid electron‐deficient cavity. Moreover, host‐guest recognition phenomena are observed between 7 and ferrocene, forming host‐guest complexes with a 1:1 stoichiometry in MeCN. 7 exhibits good redox properties, narrow energy gaps, and strong absorption in the visible range (370‐500 nm) due to containing two selenoviologen (SeV2+) units. Meanwhile, the femtosecond transient absorption (fs‐TA) reveals that 7 has stabilized dicationic biradical, efficient charge separation, and facilitates directional electron flow to achieve efficient electron transfer due to the formation of rigid cyclophane and electronic architecture. Then, 7 is applied to visible‐light‐driven hydrogen evolution with high hydrogen production (132 μmol), generation rate (11 μmol/h), turnover number (221), and apparent quantum yield (1.7%), which provides a simplified and efficient photocatalytic strategy for solar energy conversion.
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