异质结
光催化
材料科学
石墨氮化碳
磷钨酸
光致发光
化学工程
半导体
氮化碳
催化作用
纳米技术
光电子学
化学
有机化学
工程类
作者
Xiaoyi Jiang,Zhenyi Zhang,Menghan Sun,Weizhen Liu,Jindou Huang,Haiyang Xu
标识
DOI:10.1016/j.apcatb.2020.119473
摘要
Rational assembly of small-sized photosensitizers onto 2D semiconductors can effectively promote the photocatalytic activity of the formed 2D heterojunction photocatalyst due to the hetero-interfacial charge-transfer process. However, the achievement of the 2D semiconductor-based heterojunction photocatalyst with the exposures of both abundant light-harvesting and catalytic sites at the hetero-interface region is still a huge challenge. Herein, we synthesized phosphotungstic acid/graphitic carbon nitride (HPW/g-C3N4) heterojunction nanosheets (NSs) with the highly-dispersed distribution of ultra-small HPW clusters (1∼2 nm) by using a facile self-assembly method based on the static adsorption-deposition process. The formed molecular-scale hetero-interface between HPW clusters and g-C3N4 NSs resulted in the exposure of abundant active-sites on the highly-dispersed HPW/g-C3N4 hetero-interface. By combining the steady-state and transient photoluminescence spectra with the wavelength-controlled experiments, we demonstrated that the hetero-interfacial charge-transfer process occurring in the HPW/g-C3N4 heterojunction NSs obeyed the Z-scheme mechanism rather than the common “type-II” heterojunction mechanism. In this way, the lifetimes of photoinduced electrons on the conduction band of g-C3N4 could be prolonged for initiating the photocatalytic solar-to-fuels conversion. Upon interband excitations of both the two hetero-components in the HPW/g-C3N4 heterojunction NSs, the photocatalytic activities of H2 generation and CO2 reduction could be enhanced by ∼2.2 and ∼6.7 times as compared to the pure g-C3N4 NSs, even though the HPW component was photocatalytic-inert for either H2 generation or CO2 reduction upon UV–vis light irradiation.
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