Atomically dispersed cobalt on quinacridone-embedded donor-acceptor conjugated mesoporous polymer for efficient photocatalytic CO2-to-syngas

Artificial photocatalytic CO2 into syngas with a suitable CO/H2 ratio for Fischer-Tropsch synthesis is a promising path toward the carbon neutrality and sustainable development, but the sluggish charge kinetics of the current catalyst systems impedes its efficiency. Herein, we report a series of cobalt single-atom photocatalysts (Co-CMP-qaDA), single Co atoms anchored on quinacridone (QA)-embedded donor-acceptor (D-A) conjugated mesoporous polymer (CMP) support by regulating the feed molar ratio of triphenylamine (donor) to triazine (acceptor) units, which show efficient CO2-to-syngas with CO/H2 ratios of 1:1.4–1:1.6. It reveals that Co-CMP-qaDA1/3 with monomer feed ratio of 1:3 shows a minimized exciton binding energy and favorable hydrophilicity, effectively promoting charge separation/transfer and proton transfer to the Co catalytic sites for accelerating *COOH-to-*CO conversion and water dissociation. A high syngas yield rate of 13.2 mmol g−1 h−1 with CO/H2 ratio of 1:1.5 is achieved, exceeding most of the currently reported single-atom photocatalysts. These QA-embedded D-A conjugated polymers open up a new avenue for tailor-made supports assisting in single-atom catalysts toward efficient photocatalytic energy conversion and environmental remediation. [Display omitted] •Atomically dispersed Co on QA-embedded donor-acceptor CMPs was developed.•Syngas production of Co-CMP-qaDA was tuned by tailoring QA-embedded D-A CMP supports.•Co-CMP-qaDA with a donor-to-acceptor feed ratio of 1:3 showed best syngas yield rate.