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Zero-dimensional g-CNQDs Coordinated Two-dimensional Porphyrin MOF Hybrids for Boosting Photocatalytic CO2 Reduction.

It is urgent yet challenging to develop photocatalysts for visible light driven CO2 reduction with high efficiency and selectivity. Here, we report a novel hybrid catalyst by coordinating zero-dimensional (0D) carbon nitride quantum dots (g-CNQDs) with two-dimensional (2D) ultrathin porphyrin MOF (PMOF). Different from previously reported hybrid catalysts combined through physical or electrostatic interaction, in our prepared g-CNQDs/PMOF hybrids, g-CNQDs are coordinated with Co active sites in PMOF, which significantly shorten the migrating pathway of both photogenerated charge carriers and gaseous substrates from g-CNQDs to Co active centers. The resulted efficient electron-hole pairs separation and long-lived trapped electrons at Co centers not only boost the photocatalytic CO2 reduction activity, but also improve its selectivity for eight-electron reduced product CH4. To our knowledge, this is the first example of hybrid catalyst combined through coordination interaction. Remarkably, the prepared hybrid catalyst exhibits a 2.34-fold enhancement in CO generation rate (16.10 μmol g-1 h-1) and a 6.02-fold enhancement in CH4 evolution rate (6.86 μmol g-1 h-1) compared to bare PMOF.