Rao Wei, Yuan Jiamin, Tang Xiaomin, Lin Kaifeng, Xu Xianzhu, Xia Hongqiang, Jiang Yanqiu, Zheng Anmin, Liu Zhiqiang
School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 15000, P.R. China.
State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Key Laboratory of Magnetic Resonance in Biological Systems, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, P.R. China.
J Phys Chem Lett. 2022 Mar 31;13(12):2808-2813. doi: 10.1021/acs.jpclett.2c00285. Epub 2022 Mar 23.
Effective contact and collision between reactants and active sites are essential for heterogeneous catalysis. Herein, we investigated molecular diffusion in more than 200 kinds of zeolites, and an intriguing "diffusive skin effect" was observed, whereby molecules migrated along the pore walls of zeolites (, diffusion trajectories) because of the effect of the guest-host interaction and diffusion barrier. Furthermore, it was found that such a "diffusive skin effect" of zeolites would strongly promote the contacts and collisions between reactants and active sites in the reaction process, which might effectively promote the zeolite-catalyzed performance. These new findings will provide some new fundamental understanding of zeolite catalytic mechanisms under confinement effect.
反应物与活性位点之间的有效接触和碰撞对于多相催化至关重要。在此，我们研究了200多种沸石中的分子扩散，并观察到一种有趣的“扩散皮肤效应”，即由于客体-主体相互作用和扩散势垒的影响，分子沿着沸石的孔壁迁移（扩散轨迹）。此外，发现沸石的这种“扩散皮肤效应”会在反应过程中强烈促进反应物与活性位点之间的接触和碰撞，这可能有效地促进沸石催化性能。这些新发现将为限域效应下沸石催化机理提供一些新的基础认识。
