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Abstract
Mimicking natural photosynthesis to convert CO
2
with H
2
O into value-added fuels achieving overall reaction is a promising way to reduce the atmospheric CO
2
level. Casting the catalyst of two or more catalytic sites with rapid electron transfer and interaction may be an effective strategy for coupling photocatalytic CO
2
reduction and H
2
O oxidation. Herein, based on the MOF
∪
COF collaboration, we have carefully designed and synthesized a crystalline hetero-metallic cluster catalyst denoted MCOF-Ti
6
Cu
3
with spatial separation and functional cooperation between oxidative and reductive clusters. It utilizes dynamic covalent bonds between clusters to promote photo-induced charge separation and transfer efficiency, to drive both the photocatalytic oxidative and reductive reactions. MCOF-Ti
6
Cu
3
exhibits fine activity in the conversion of CO
2
with water into HCOOH (169.8 μmol g
−1
h
−1
). Remarkably, experiments and theoretical calculations reveal that photo-excited electrons are transferred from Ti to Cu, indicating that the Cu cluster is the catalytic reduction center.