The g-C_3N_4 with different structures was prepared by heat treatment using urea(CN-U) and thiourea(CN-T) as precursors under the same conditions. The microstructure and optical properties of the photocatalyst were an...The g-C_3N_4 with different structures was prepared by heat treatment using urea(CN-U) and thiourea(CN-T) as precursors under the same conditions. The microstructure and optical properties of the photocatalyst were analyzed with advanced tools. The results showed that the CN-U has a porous structure, a high specific surface area and a wide band gap in comparison with CN-T. The in situ FT-IR technique was used to monitor the adsorption and reaction process of visible photocatalytic NO oxidation on g-C_3N_4. The corresponding reaction mechanism was proposed based on the results of reaction intermediate observation and electron paramagnetic resonance(EPR) radical scavenging. It was revealed that(1) the presence of defective sites favored the adsorption of gas molecules and electronically compensated it leading to promoted formation of the final products;(2) the high separation efficiency of photogenerated electron-hole pairs enhanced the production of radicals during the photocatalytic reaction;(3) the hydroxyl radicals(-OH) are not selective for the decomposition of pollutants, which are favorable to the complete oxidation of the reaction intermediates. The above three aspects are the main reasons for the CN-U possessing the efficient visible light photocatalytic activity. The present work could provide new insights and methods for understanding the mechanism of photocatalysis.展开更多
基金supported by the National Key Research and Development Plan (2016YFC02047)the National Natural Science Foundation of China (51478070, 21777011 and 21501016)+1 种基金the Innovative Research Team of Chongqing (CXTDG201602014)the Natural Science Foundation of Chongqing (cstc2017jcyj BX0052, cstc2016jcyj A0481)
文摘The g-C_3N_4 with different structures was prepared by heat treatment using urea(CN-U) and thiourea(CN-T) as precursors under the same conditions. The microstructure and optical properties of the photocatalyst were analyzed with advanced tools. The results showed that the CN-U has a porous structure, a high specific surface area and a wide band gap in comparison with CN-T. The in situ FT-IR technique was used to monitor the adsorption and reaction process of visible photocatalytic NO oxidation on g-C_3N_4. The corresponding reaction mechanism was proposed based on the results of reaction intermediate observation and electron paramagnetic resonance(EPR) radical scavenging. It was revealed that(1) the presence of defective sites favored the adsorption of gas molecules and electronically compensated it leading to promoted formation of the final products;(2) the high separation efficiency of photogenerated electron-hole pairs enhanced the production of radicals during the photocatalytic reaction;(3) the hydroxyl radicals(-OH) are not selective for the decomposition of pollutants, which are favorable to the complete oxidation of the reaction intermediates. The above three aspects are the main reasons for the CN-U possessing the efficient visible light photocatalytic activity. The present work could provide new insights and methods for understanding the mechanism of photocatalysis.