English
The photocatalytic conversion of CO2 into valuable hydrocarbon fuels has broad prospects in addressing emerging energy shortages and environmental crises while meeting urgent social and national development needs. However, its efficiency is hindered by limited CO2 chemical adsorption, rapid electron hole recombination, and weak redox ability. Inspired by the unique characteristics of the Schiff covalent organic framework (COF), including a large specific surface area, unique pore structure, and abundant weakly basic nitrogen elements, we use TPA-COF to enhance the chemical adsorption and activation of acidic substances. CO2 molecules were validated through CO2 programmed temperature desorption analysis. In addition, anchoring CsPbBr3 quantum dots (QDs) onto COFs facilitates effective spatial separation of photo generated charge carriers with strong redox capabilities, as evidenced by the formation of an S-shaped heterojunction between COFs and QDs, as confirmed by in-situ X-ray irradiation using photoelectron spectroscopy, femtosecond transient absorption spectroscopy, and density functional theory simulations. As expected, the optimized COF/QD heterostructure exhibited significantly enhanced CO2 photoreduction performance without any molecular co catalysts or scavengers, with CO and CH4 production rates of 41.2 and 13.7 μ mol g-1, respectively. This work provides valuable insights into the development of novel organic/inorganic heterojunction photocatalysts with CO2 chemical adsorption and S-type charge separation, offering enormous potential for sustainable artificial photosynthesis.
