Regulating Utilization Efficiency of the Photogenerated Charge Carriers by Constructing Donor-π-Acceptor Polymers for Upgrading Photocatalytic CO2 Reduction.

Photocatalytic CO2 reduction offers a promising approach for managing global carbon balance. The smooth delivery of the photoexcited electrons to the active sites without the extra photosensitizers is still challenging. Herein, a series of donor-π-acceptor conjugated organic polymers (COPs) were produced using anthracene, cobalt-coordinated bipyridyl, and benzene as donor, acceptor, and π linker units, respectively. The introduction of phenyl linker significantly improved the activities of photocatalytic CO2 reduction upon visible light illumination. Structure-performance relationship examinations uncovered that donor-π-acceptor structure promotes mobility of charge carriers and utilization efficiency on the catalytically active sites, resulting in high photocatalytic activity and durability for CO2 photoreduction. The in-depth insights into the electron transport processes open new perspectives for further optimization and rational design of photoactive polymers with high efficiency for solar-energy conversion.