光催化反应中表界面过程的同步辐射原位红外光谱研究

The main goal of the proposal is to investigate the reaction mechanism in the photocatalytic process by employing the synchrotron radiation infrared beamline with the strength of BL01B endstation at National Synchrotron Radiation Laboratory and National Center for Protein Science Shanghai (NCPSS) endstation at Shanghai Synchrotron Radiation Facility. With the development of photocatalytic time-resolved spectra collection technique, the integration of external and internal ATR technique, the far-infrared spectroscopy characterization method of weak-bond adsorption and metal-molecule adsorption on surfaces/interfaces, and upgraded DRIFTS technique, the comprehensive understanding of photocatalytic reaction on micro scale and in molecular level can be achieved due to the high sensitivity and high resolution of infrared spectroscopy from mid-infrared to far-infrared region. By performing in-situ detection of active sites, adsorptive substances and intermediates on surfaces/interfaces, and analyzing adsorption and weak-bonding structures, and dynamics in the typical photocatalytic processes, such as degradation of organics in aqueous, CO2 reduction, and degradation of VOCs in gaseous, the project will propose new mechanisms and clarify the controversial issues in photocatalytic reactions. Moreover, the project will offer rational design and fabrication methods in novel photocatalysts systems, establish a photocatalytic research base at synchrotron radiation infrared endstations, and promote the photocatalytic progress in the field of energy conversion and environment treatment.

依托合肥光源和上海光源，集成合肥光源红外谱学与显微成像实验站和国家蛋白质中心红外线站在中、远红外波段的优势，针对光催化反应中的典型表界面过程，配置相关原位条件，研制光催化过程时间分辨红外光谱采集的同步系统，发展内、外反射双通道ATR原位表征技术，发展表面弱键吸附、金属-分子吸附的远红外表征技术，完善DRIFTS技术，全面建立光催化表界面反应的高灵敏度、高分辨、覆盖远红外的同步辐射原位红外光谱研究方法，在微观层次和分子水平研究光催化过程。通过检测光催化降解液相有机污染物（固液）、还原CO2（固液/固气）、降解VOCs（固气）等过程中表界面上的关键物种（表面活性位、活性物种、吸附物种与构型、弱键构型、中间产物等），提出和澄清相关反应机理，形成对光催化反应过程的全面认识，指导光催化的新型表界面体系设计与构建，达到理性设计光催化材料、控制反应过程，推动光催化能源与环境相关学科的发展。

项目依托合肥光源和上海光源红外实验站，针对光催化反应中的典型表界面过程，配置了相关原位条件，发展了一系列用于光催化表界面反应机理研究的高灵敏度、高分辨、覆盖远红外的同步辐射原位红外光谱研究方法。结合典型光催化研究，在微观层次和分子水平探索了光催化降解污染物、还原CO2、分解水制氢等过程，对关键物种（表面活性位、活性物种、吸附物种与构型、弱键构型、中间产物等）进行了定性和定量分析，提出和澄清了一些反应机理，形成了对光催化反应过程的较全面认识。项目实施为光催化的新型表界面体系设计与构建提供了指导，推动了光催化能源与环境相关学科的发展。共计发表论文27篇，申请专利3项，软件著作权1项，培养博士后1名，研究生6名。