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S-scheme heterojunction of crystalline carbon nitride nanosheets and ultrafine WO3 nanoparticles for photocatalytic CO2 reduction

氮化碳 光催化 材料科学 异质结 化学工程 纳米颗粒 氮化物 催化作用 吸附 纳米技术 化学 光电子学 有机化学 图层(电子) 工程类
作者
Gongjie Chen,Ziruo Zhou,Bifang Li,Xiahui Lin,Can Yang,Yuanxing Fang,Wei Lin,Yidong Hou,Guigang Zhang,Sibo Wang
出处
期刊:Journal of Environmental Sciences-china [Elsevier]
被引量:77
标识
DOI:10.1016/j.jes.2023.05.028
摘要

Highly crystalline carbon nitride polymers have shown great opportunities in overall water photosplitting; however, their mission in light-driven CO2 conversion remains to be explored. In this work, crystalline carbon nitride (CCN) nanosheets of poly triazine imide (PTI) embedded with melon domains are fabricated by KCl/LiCl-mediated polycondensation of dicyandiamide, the surface of which is subsequently deposited with ultrafine WO3 nanoparticles to construct the CCN/WO3 heterostructure with a S-scheme interface. Systematic characterizations have been conducted to reveal the compositions and structures of the S-scheme CCN/WO3 hybrid, featuring strengthened optical capture, enhanced CO2 adsorption and activation, attractive textural properties, as well as spatial separation and directed movement of light-triggered charge carriers. Under mild conditions, the CCN/WO3 catalyst with optimized composition displays a high photocatalytic activity for reducing CO2 to CO in a rate of 23.0 µmol/hr (i.e., 2300 µmol/(hr*g)), which is about 7-fold that of pristine CCN, along with a high CO selectivity of 90.6% against H2 formation. Moreover, it also manifests high stability and fine reusability for the CO2 conversion reaction. The CO2 adsorption and conversion processes on the catalyst are monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), identifying the crucial intermediates of CO2*−, COOH* and CO*, which integrated with the results of performance evaluation proposes the possible CO2 reduction mechanism.
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