化学吸附
光诱导电荷分离
异质结
人工光合作用
量子点
材料科学
X射线光电子能谱
光催化
化学
光化学
化学工程
纳米技术
催化作用
光电子学
有机化学
工程类
作者
Ying He,Peiyu Hu,Jianjun Zhang,Guijie Liang,Jiaguo Yu,Feiyan Xu
标识
DOI:10.1021/acscatal.4c00026
摘要
Photocatalytic conversion of CO2 into valuable hydrocarbon fuels holds great promise in addressing emerging energy shortages and environmental crises while fulfilling pressing societal and national development demands. Nonetheless, its efficiency is hindered by restricted CO2 chemisorption, rapid electron–hole recombination, and weak redox capability. Drawing inspiration from the distinctive characteristics of Schiff-based covalent organic frameworks (COFs), including substantial specific surface area, unique pore structure, and an abundance of weakly alkaline nitrogen elements, we employ the TPA-COF to enhance the chemisorption and activation of acidic CO2 molecules, as validated by the CO2-temperature-programmed desorption analysis. Furthermore, anchoring CsPbBr3 quantum dots (QDs) onto the COF facilitates the effective spatial separation of photoinduced charge carriers with strong redox capability, resulting from the formation of S-scheme heterojunctions between the COF and QDs as substantiated by in situ irradiation X-ray photoelectron spectroscopy, femtosecond transient absorption spectroscopy, and density functional theory simulations. As anticipated, the optimized COF/QDs heterostructures exhibit remarkable enhancements in CO2 photoreduction performance in the absence of any molecule cocatalyst or scavenger, yielding CO and CH4 at rates of 41.2 and 13.7 μmol g–1, respectively. This work provides valuable insights into the development of novel organic/inorganic heterojunction photocatalysts with CO2 chemisorption and S-scheme charge separation, offering great potential for sustainable artificial photosynthesis.
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