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作 者:Gongjie Chen Ziruo Zhou Bifang Li Xiahui Lin Can Yang Yuanxing Fang Wei Lin Yidong Hou Guigang Zhang Sibo Wang
出 处:《Journal of Environmental Sciences》2024年第6期103-112,共10页环境科学学报(英文版)
基 金:supported by the National Key R&D Program of China(Nos.2021YFA1502100 and 2022YFE0114800);the National Natural Science Foundation of China(Nos.22311540011 and 21973014)。
摘 要:Highly crystalline carbon nitride polymers have shown great opportunities in overall water photosplitting;however,their mission in light-driven CO_(2)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 WO_(3)nanoparticles to construct the CCN/WO_(3)heterostructure with a S-scheme interface.Systematic characterizations have been conducted to reveal the compositions and structures of the S-scheme CCN/WO_(3)hybrid,featuring strengthened optical capture,enhanced CO_(2)adsorption and activation,attractive textural properties,as well as spatial separation and directed movement of light-triggered charge carriers.Under mild conditions,the CCN/WO_(3)catalyst with optimized composition displays a high photocatalytic activity for reducing CO_(2)to CO in a rate of 23.0μmol/hr(i.e.,2300μmol/(hr·g)),which is about 7-fold that of pristine CCN,along with a high CO selectivity of 90.6%against H2formation.Moreover,it also manifests high stability and fine reusability for the CO_(2)conversion reaction.The CO_(2)adsorption and conversion processes on the catalyst are monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS),identifying the crucial intermediates of CO_(2)^(*)-,COOH^(*)and CO^(*),which integrated with the results of performance evaluation proposes the possible CO_(2)reduction mechanism.
关 键 词:Crystalline carbon nitride Photocatalysis CO_(2)reduction S-scheme WO_(3)
分 类 号:X701[环境科学与工程—环境工程]
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