Zhang Zhen-Yu, Xie Tao
Institute of Industrial Catalysis, School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, PR China.
Institute of Industrial Catalysis, School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, PR China.
J Colloid Interface Sci. 2025 Jan;677(Pt A):863-872. doi: 10.1016/j.jcis.2024.08.019. Epub 2024 Aug 5.
Solar-driven photo-thermal dry reforming of methane (DRM) is an environmentally friendly production route for high-value-added chemicals. However, the lack of thorough understanding of the mechanism for photo-thermal reaction has limited its further development. Here, we systematically investigated the mechanism of photo-thermal DRM reaction with the representative of Ru/CeO catalyst. Through in situ DRIFTs and transient experiments, comprehensive investigation into the reaction steps and their reactive sites in the process of DRM reaction were conducted. Besides, the excitation and migration direction of photo-electron was determined by ISI-XPS experiments, and the change of surface defect structure induced by light was characterized by ISI-EPR experiments. Based on the above results, the photo-enhancement effect on each micro-reaction step was determined. This study provides a theoretical basis for the industrialization of photo-thermal DRM reaction and its development of catalysts.
太阳能驱动的甲烷光热干重整（DRM）是一种生产高附加值化学品的环境友好型路线。然而，对光热反应机理缺乏深入了解限制了其进一步发展。在此，我们以Ru/CeO催化剂为代表，系统地研究了光热DRM反应的机理。通过原位漫反射红外傅里叶变换光谱（DRIFTs）和瞬态实验，对DRM反应过程中的反应步骤及其反应位点进行了全面研究。此外，通过离子散射诱导X射线光电子能谱（ISI-XPS）实验确定了光电子的激发和迁移方向，通过离子散射诱导电子顺磁共振（ISI-EPR）实验表征了光诱导的表面缺陷结构变化。基于上述结果，确定了光对各微反应步骤的增强作用。本研究为光热DRM反应的工业化及其催化剂的开发提供了理论依据。
