A strategy to covalently connect crystalline covalent organic frameworks (COFs) with semiconductors to create stable organic-inorganic Z-scheme heterojunctions for artificial photosynthesis is presented. A series of COF-semiconductor Z-scheme photocatalysts combining water-oxidation semiconductors (TiO , Bi WO , and α-Fe O ) with CO reduction COFs (COF-316/318) was synthesized and exhibited high photocatalytic CO -to-CO conversion efficiencies (up to 69.67 μmol g h ), with H O as the electron donor in the gas-solid CO reduction, without additional photosensitizers and sacrificial agents. This is the first report of covalently bonded COF/inorganic-semiconductor systems utilizing the Z-scheme applied for artificial photosynthesis. Experiments and calculations confirmed efficient semiconductor-to-COF electron transfer by covalent coupling, resulting in electron accumulation in the cyano/pyridine moieties of the COF for CO reduction and holes in the semiconductor for H O oxidation, thus mimicking natural photosynthesis.
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