期刊
ACS APPLIED MATERIALS & INTERFACES
卷 11, 期 45, 页码 42243-42249出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b15306
关键词
photocatalysts; CO2 reduction; zero-dimensional g-CNQDs; two-dimensional porphyrin MOF; 0D/2D hybrid catalysts
资金
- National Natural Science Foundation of China [21874018, 21635004, 21627806, 21705018]
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 (OD) 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 interactions, in our prepared g-CNQDs/PMOF hybrids, g-CNQDs are coordinated with Co active sites in PMOF, which significantly shortens the migrating pathway of both photogenerated charge carriers and gaseous substrates from g-CNQDs to Co active centers. The resulting efficient electron-hole pair separation and long-lived trapped electrons at Co centers not only boost the photocatalytic CO, reduction activity but also improve its selectivity for the eight-electron reduced product CH4. To our knowledge, this is the first example of a hybrid catalyst combined through coordination interaction. Remarkably, the prepared hybrid catalyst exhibits a 2.34-fold enhancement in the CO generation rate (16.10 mu mol g(-1) h(-1)) and a 6.02-fold enhancement in the CH4 evolution rate (6.86 mu mol g(-1) h(-1)) compared to the bare PMOF.
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