单晶异面选择性沉积Pt-TiO2光催化还原湿CO2的反应机理

Photocatalytic conversion of CO2 into hydrocarbon fuels has great value to solve the global warming and the lack of energy. The proposal project is going to focus on this hot issue. TiO2 nanocrystals with Pt selective deposition on {101}/{001} facets will be synthesized by a solvothermal method coupled with a photodeposition method, and will be characterized systematically by Rietveld refinement method using several analysis equipments. The photocatalytic activity of the catalyst and the selectivity of the products will be quantitatively evaluated by an online continuous flow reactor system and the effects of flue gas composition and reaction condition on the photocatalytic process will be analyzed. The evolution of surface interfacial properties of catalyst in simulated wet CO2 flue gas will be explored, which is helpful for the optimization of the preparation of catalyst. The CO2 catalytic conversion mechanism by Pt-TiO2{101}/{001} will be revealed, and the economy and environmental effects of the technology will be evaluated based on life cycle assessment. The results of the project will provide the theoretical basis for the large-scale development and application of photocatalytic conversion of oxyfuel combustion flue gas into hydrocarbon fuels.

利用人工光合作用为路径将CO2直接光催化还原制取CH燃料，既能减排温室气体又能获得化工原料，对于从根本上解决由CO2带来的气候变化及能源危机均具有重大意义。本项目将构建一种新型TiO2单晶异面{101}/{001}选择性沉积Pt的催化剂(Pt-TiO2)，借助Rietveld全谱拟合精修对其晶面结构特征进行精细表征；并对Pt-TiO2直接光催化转化湿CO2模拟烟气活性及产物选择性进行定量评价；分析反应工况及模拟烟气中典型组分等对光催化过程的影响，探究催化剂表界面特性在湿CO2模拟烟气中的演化规律，优化Pt-TiO2催化剂的设计制备方法，揭示Pt-TiO2对湿CO2模拟烟气的定向转化机制；并采用全生命周期评价方法对新型湿CO2模拟烟气直接光催化转化系统的经济性及环境效益进行评价，以期建立湿CO2烟气直接光催化转化制CH燃料方法，为探寻烟气CO2直接高值化利用新方法提供理论基础和技术支撑。

利用人工光合作用为路径将CO2直接光催化还原制取CH燃料，既能减排温室气体又能获得化工原料，对于从根本上解决由CO2带来的气候变化及能源危机均具有重大意义。本项目开发一种新型TiO2单晶异面{101}/{001}选择性沉积Pt的催化剂(Pt-TiO2)，借助Rietveld全谱拟合精修对其晶面结构特征进行了精细表征；对Pt-TiO2直接光催化转化湿CO2模拟烟气活性及产物选择性进行了定量评价；分析了反应工况等对光催化过程的影响，揭示了Pt-TiO2对湿CO2烟气的定向转化机制，建立了Pt-TiO2光催化转化湿CO2模拟烟气的反应动力学模型，在此基础上优化Pt-TiO2催化剂的设计制备方法；采用全生命周期评价方法对湿 CO2 模拟烟气直接光催化燃料化过程进行了系统环境经济评价和优化，为实现烟气CO2直接高值化利用提供理论基础和技术支撑。