Poly(heptazine imide) (PHI), one of the crystalline or long-range ordered allotropes of polymeric carbon nitride, is a promising polymeric photocatalyst; however, preparation of highly crystalline PHI remains a challenge. Herein, through a bottom-up strategy involving repair of structural defects and increase of specific surface area of melon precursor, we prepared PHI nanorods with dramatically improved long-range order. The resulting PHI exhibited a shift of product selectivity in CO photoreduction from CO to CH with a high methanation activity in contrast to the pristine PHI with relatively low long-range order.
View Article and Find Full Text PDFCu-based catalysts have been shown to selectively catalyze CO photoreduction to C solar fuels. However, they still suffer from poor activity and low selectivity. Herein, we report a high-performance carbon nitride supported Cu single-atom catalyst featuring defected low-coordination Cu-N motif (Cu-N-V).
View Article and Find Full Text PDFThe in-plane heterojunctions with atomic-level thickness and chemical-bond-connected tight interfaces possess high carrier separation efficiency and fully exposed surface active sites, thus exhibiting exceptional photocatalytic performance. However, the construction of in-plane heterojunctions remains a significant challenge. Herein, we prepared an in-plane ZnInS/In(OH) heterojunction (ZISOH) by partial conversion of ZnInS to In(OH) through the addition of HO.
View Article and Find Full Text PDFPhotoreduction of CO to C solar fuel is a promising carbon-neutral technology for renewable energy. This strategy is challenged by its low productivity due to low efficiency in multielectron utilization and slow C-C coupling kinetics. This work reports a dual-metal photocatalyst consisting of atomically dispersed indium and copper anchored on polymeric carbon nitride (InCu/PCN), on which the photoreduction of CO delivered an excellent ethanol production rate of 28.
View Article and Find Full Text PDFFundamental photocatalytic limitations of solar CO reduction remain due to low efficiency, serious charge recombination, and short lifetime of catalysts. Herein, two-dimensional graphitic carbon nitride nanosheets with nitrogen vacancies (g-C N ) located at both three-coordinate N atoms and uncondensed terminal NH species were prepared by one-step tartaric acid-assistant thermal polymerization of dicyandiamide. Transient absorption spectra revealed that the defects in g-C N act as trapped states of charges to result in prolonged lifetimes of photoexcited charge carriers.
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