上海市磁共振重点实验室

叶曼等同学于Journal of Catalysis上发表文章

发布日期: 2019-10-16   作者:   浏览次数: 135

近日,本实验室叶曼以及徐贝贝等同学于《Journal of Catalysis》上发表了题为《Probing the methanol heterogeneous photochemistry processes by operando NMR – The role of bulk water

》的文章。(https://doi.org/10.1016/j.jcat.2019.08.016


Abstract

Solid-liquid heterogeneous catalysis reactions play key roles in industrial catalytic reactions, throughout pollution control, fuel cell, methanol reforming and so on. But, few operando techniques have been performed to track the complex reaction processes, especially those in bulk liquid environment containing two or more liquid reactants, thus leaving a gap in our understanding of the reaction mechanisms deep into the working conditions. Here, we demonstrate an approach, using operando nuclear magnetic resonance (NMR) to probe the dynamics and kinetics of the methanol heterogeneous photochemistry processes in liquid condition with and without bulk water (H2O). It shows that not only can bulk H2O affect the types of methanol reforming products, but also its participation way can vary from H2O molecule to H-atom. Furthermore, the productivities of the main products - methylene glycol (HOCH2OH) and hemiacetal (CH3OCH2OH) – show different dependency on the H2O concentration, which is further supported by the density functional theory calculations (DFT). The operando NMR method opens up exciting opportunities for the mechanism studies of heterogeneous catalysis reaction in bulk liquid.