Intermolecular cascaded π-conjugation channels for electron delivery powering CO<sub>2</sub> photoreduction.

Wang, Shengyao; Hai, Xiao; Ding, Xing; Jin, Shangbin; Xiang, Yonggang; Wang, Pei; Jiang, Bo; Ichihara, Fumihiko et al. · Nat Commun · 2020

basic_science · Level V

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Abstract

Photoreduction of CO<sub>2</sub> to fuels offers a promising strategy for managing the global carbon balance using renewable solar energy. But the decisive process of oriented photogenerated electron delivery presents a considerable challenge. Here, we report the construction of intermolecular cascaded π-conjugation channels for powering CO<sub>2</sub> photoreduction by modifying both intramolecular and intermolecular conjugation of conjugated polymers (CPs). This coordination of dual conjugation is firstly proved by theoretical calculations and transient spectroscopies, showcasing alkynyl-removed CPs blocking the delocalization of electrons and in turn delivering the localized electrons through the intermolecular cascaded channels to active sites. Therefore, the optimized CPs (N-CP-D) exhibiting CO evolution activity of 2247 μmol g<sup>-1</sup> h<sup>-1</sup> and revealing a remarkable enhancement of 138-times compared to unmodified CPs (N-CP-A).