光电联合催化CO2还原反应中有机/无机半导体薄膜界面工程调控光阴极促进光生电荷分离及传输的研究

The efficiency of photoelectrocatalytic (PEC) CO2 reduction is limited by the series recombination of photogenerated charges, high overpotential and sluggish kinetics of surface reaction. So, the rational design of photocathode architecture for efficient PEC CO2 reduction still remains a key bottleneck. Considering different recognition and transportation ability of semiconductor for electrons and holes, the project proposed charge transport layers as energy ladder have been introduced to overcome charge injection or extraction barriers based on the original semiconductor material and achieve the effective separation of photogenerated charge carriers and selective transmission. According to the above purposes, we will prepare the photocathode with FTO/HTL/Pn/M and FTO/HTL/BHJ/M to study the relationship between the microstructure and the separation and transmission of photo-generated charge. The implementation of this project is expected to solve the problem of interfacial charge recombination and inefficient photogeneration carrier collection on traditional photocatalyst. It may promote the application of various types of semiconductor materials to the construction of photocathode.

光电催化二氧化碳还原的性能一直受到光生电荷的复合，电位高以及表面还原反应的发生困难等条件的制约。合理设计光阴极体系结构，仍然是一个关键的瓶颈。本项目提出利用半导体对电子和空穴的不同识别及运转能力，在原有光催化半导体的基础上构建电荷传输层，并提供能量阶梯，从而克服光材料电荷注入和提取的能垒，达到有效分离光生电荷和选择性传输载流子的目的。基于以上理解，制备出具有FTO/HTL/Pn/M和FTO/HTL/BHJ/M多种形貌、多层功能界面结构的光催化剂，并研究光阴极的微观结构和光生电荷分离及传输之间的关系。本项目的实施有望解决传统光催化剂界面电荷复合、光生载流子收集效率低的问题，并推动各种类型的半导体材料应用到光阴极结构的构建。

光电催化还原反应的性能一直受到光生电荷的复合，电位高以及表面还原反应的发生困难等条件的制约。合理设计光阴极体系结构仍然是一个关键的瓶颈。本项目关注多功能薄膜在构建高效光阴极催化体系发挥的重要作用，通过调控对电子和空穴的不同识别及运转能力的半导薄膜，获得催化性能最佳的光阴极。通过本项目的实施，明确了多功能薄膜在优化光生电荷分离而所作出的重要作用。多功能薄膜在构建高效光阴极参与光电联合催化的方面具有显著效果。本项目的顺利推进和完成，提供了构建新型优越光阴极方案，且有助于推向光阴极参与反应的各个领域。