4.8 Article

Engineering cuboctahedral N-doped C-coated p-CuO/n-TiO2 heterojunctions toward high-performance photocatalytic cross-dehydrogenative coupling

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NANOSCALE
卷 15, 期 32, 页码 13313-13321

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ROYAL SOC CHEMISTRY
DOI: 10.1039/d3nr00717k

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A cuboctahedral N-doped carbon-coated CuO/TiO2 p-n heterojunction was designed and fabricated successfully for the first time, demonstrating enhanced transport and separation of photoinduced e-h pairs. The nitrogen-doped carbon coating plays a pivotal role in promoting the overall performance and effectiveness of the reaction. The CuO-TiO2@N-C exhibits superior photocatalytic efficiency, cycle stability and substrate scope towards cross-dehydrogenative coupling reactions.
The low separation efficiency of photogenerated electron-hole (e-h) pairs severely limits the activation of photocatalyts. One brilliant strategy is to construct a p-n type semiconductor heterojunction, which can establish an inner electric field to separate the e-h pairs with high efficiency. Here, for the first time, a cuboctahedral N-doped carbon-coated CuO/TiO2 p-n heterojunction (CuO-TiO2@N-C) was designed and fabricated successfully via direct calcination of a benzimidazole-modulated cuboctahedral HKUST-Cu with titanium-tetraisopropanolate absorbed inside concomitantly. Full structural characterizations incorporating DFT computations demonstrate that the CuO/TiO2 p-n heterostructure can greatly boost the transport and separation of photoinduced e-h pairs. The nitrogen-doped carbon coating, with its excellent conductivity, porosity, stability and surface reaction activity, plays a pivotal role in promoting the overall performance and effectiveness of the reaction. The CuO-TiO2@N-C displays significantly higher photocurrent density (0.042 & mu;A cm(-2)) than the CuO@N-C (0.014 & mu;A cm(-2)) and TiO2@N-C (0.03 & mu;A cm(-2)) electrodes, proving that the p-n heterojunction can improve the e-h generation efficiency. This unique photocatalyst affords superior photocatalytic efficiency, cycle stability and substrate scope towards cross-dehydrogenative coupling reactions.

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