铁酸盐/生物酶偶合仿生催化体系的构建及其酶促光催化还原CO2性能的研究

Carbon dioxide (CO2) is one of the main greenhouse gases in global environment, which can cause serious harm to the future environment for human survival and the Earth's ecosystem. Thus, how to effectively reduce or convert the atmospheric CO2 is a very important subject in the current academic field of environment science. The submitted proposal aims at improving photocatalytic conversion efficiency of the greenhouse gas molecules CO2 by building MFe2O4 /Bio-Enzyme (M = Ca, Mg, etc.; BE = CODH, FDH, etc.) coupling biomimic catalytic material at the molecular level to promote the separation and migration of photogenerated carriers, in order to achieve further enhanced efficiency of photocatalytic activation and reduction of CO2. Furthermore, isotope-labeled probe technology with a variety of online spectral means will be employed to comprehensively study the reaction mechanisms at the molecular level to understand the microscopic mechanisms of photo-induced charges behavior in the catalytic system, and the processes of adsorption, activation, reduction and desorption of CO2 molecules at the catalyst surface or interface. The implementation of this project will provide people with deep insights into the properties of enzymatic and photocatalytic reduction of the CO2 molecule under complex reaction conditions, which has extremely important practical significance and reference value for abatement, control and resource utilization of CO2, the greenhouse gas.

二氧化碳（CO2）是主要的大气环境温室气体之一，对人类未来的生存环境和地球的生态系统造成严重危害, 因此如何有效消减及转化大气中的CO2是当今环境领域的重大课题。本申请项目以提高CO2温室气体分子光助催化转化效率为研究目标，通过在分子水平上构建MFe2O4/Bio-Enzyme (M=Ca, Mg, etc.; BE=CODH, FDH, etc.)偶合仿生催化材料，促进光生载流子的分离效率与迁移速率，从而实现CO2催化活化与还原转化效率的进一步提高。拟采用同位素标记分子探针技术结合多种原位在线谱学手段深入研究有关反应机理，从分子水平上理解体系中的光致电荷行为，揭示CO2分子在催化剂表面-界面的吸附、活化、还原及脱附微观过程机制。本项目的实施将深化人们对温室气体CO2分子在复杂反应条件下酶促光催化还原特性的认识，对CO2温室气体的消减控制和资源化利用具有重要的参考价值与现实意义。

对二氧化碳(CO2) 温室气体的消减控制和资源化利用是当今环境领域的重大课题。本项目通过在分子水平上构建AB2O4/Bio-Enzyme (A = Ni, Ca, Zn, etc.; B = Fe, Co; BE = CODH, FDH, etc.)偶合仿生催化材料，结合多种原位在线谱学手段深入研究相关反应机理，从分子水平上理解体系中的光致电荷产生及迁移的瞬态动力学过程，揭示CO2分子在催化剂表面-界面的吸附、活化、还原及脱附微观过程机制。课题在以下两个方面取得了重要进展：(1)基于湿化学技术构筑了一系列不同结构形态的MFe2O4和MCo2O4类尖晶石材料，结合厌氧条件吸附方法构建了系列具有稳定催化性能的酶助仿生催化体系，并建立该催化过程重要活性物种的原位在线检测和分析方法。(2)识别对CO2分子光催化活化、转化反应过程起关键作用的催化材料结构形态以及各类反应影响因素，阐明酶促光致催化反应产物的形成与催化材料结构形态及反应影响因素之间的相关性。相关研究成果包括SCI收录的国际重要期刊论文34篇，申请国家发明专利6项，授权专利1项。