In situ no-slot joint integration of half-metallic C(CN)3 cocatalyst into g-C3N4 scaffold: An absolute metal-free in-plane heterosystem for efficient and selective photoconversion of CO2 into CO
An absolute metal-free in-plane heterosystem consisting of g-C 3 N 4 as scaffold and embedded half-metallic C(CN) 3 as cocatalysts was conceptually designed for photoconversion of CO 2 . The no-slot joint between half-metallic C(CN) 3 and g-C 3 N 4 through covalent bonding generates a unique two-dimensional, π-conjugated hybrid structure, allowing obstacle-free transferring of the photogenerated electrons in g-C 3 N 4 into C(CN) 3 via an intrinsic driving force. Our theoretical calculations together with the in-situ Fourier transform infrared spectra indicate that the most negative charge distribution and binding energy with CO 2 for C(CN) 3 allow outstanding capture and chemical activation capacity toward CO 2 , and subsequently enable the optimized heterosystem to exhibit highly efficient and selective photocatalytic reduction of CO 2 into CO, 7.8 and 1.9 times those produced with pristine and Pt-modified g-C 3 N 4 , respectively. The no-slot joint of organic half-metal cocatalysts with g-C 3 N 4 may open up new opportunities for metal-free, polymer-based photocatalytic systems for CO 2 conversion and solar fuel generation.
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