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Photodriven charge separation is a key process for converting solar energy into chemical energy. However, it remains a challenge to develop artificial light-harvesting materials that can simultaneously achieve ultrafast charge separation and a long-lived charge-separated state with low energy loss. In contrast to conventional strategies based on covalent or noncovalent interactions, we employed a mechanical bond to forcibly assemble two strongly electron-deficient cationic chromophores (TTzBox4+ and PDI-C2+), which have very similar reduction potentials and exhibit limited noncovalent interactions, into a hetero2catenane (TTzPCat6+). This design provides efficient π electronic couplings, enabling ultrafast charge separation ( 1000), surpassing the conventional trade-off between driving force and charge separation efficiency in heterogeneous donor–acceptor systems. The photocatalytic system based on TTzPCat6+ exhibits an over 2-fold enhancement in selective oxidation of aryl sulfides under mild conditions, demonstrating the potential of mechanical bonding for preparing photocatalytic materials. This investigation not only highlights a strategy for achieving highly efficient charge separation with low energy loss but also offers fresh insights into developing efficient solar energy conversion systems.
Zhao et al. (Thu,) studied this question.