Hu Shen, Liu Junru, Ye Guanghua, Zhou Xinggui, Coppens Marc-Olivier, Yuan Weikang
State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
Department of Chemical Engineering, University College London, London, WC1E 7JE, UK.
Angew Chem Int Ed Engl. 2021 Jun 21;60(26):14394-14398. doi: 10.1002/anie.202104859. Epub 2021 May 17.
We have developed a generalizable strategy to quantify the effect of surface barriers on zeolite catalysis. Isomerization of n-pentane, catalyzed by Pt/Beta, is taken as a model reaction system. Firstly, the surface modification by chemical liquid deposition of SiO was carried out to control the surface barriers on zeolite Beta crystals. The deposition of SiO leads to a very slight change in the physical properties of Beta crystals, but an obvious reduction in Brønsted acid sites. Diffusion measurements by the zero-length column (ZLC) method show that the apparent diffusivity of n-pentane can be more than doubled after SiO deposition, indicating that the surface barriers have been weakened. Catalytic performance was tested in a fixed-bed reactor, showing that the apparent catalytic activity improved by 51-131 % after SiO deposition. These results provide direct proof that reducing surface barriers can be an effective route to improve zeolite catalyst performance deteriorated by transport limitations.
我们已经开发出一种可推广的策略来量化表面屏障对沸石催化的影响。以Pt/Beta催化正戊烷的异构化反应作为模型反应体系。首先,通过化学液相沉积SiO进行表面改性,以控制沸石Beta晶体上的表面屏障。SiO的沉积导致Beta晶体的物理性质发生非常轻微的变化,但布朗斯特酸位点明显减少。通过零长度柱(ZLC)方法进行的扩散测量表明,SiO沉积后正戊烷的表观扩散率可以增加一倍以上,这表明表面屏障已经减弱。在固定床反应器中测试了催化性能,结果表明SiO沉积后表观催化活性提高了51-131%。这些结果提供了直接证据,表明减少表面屏障可以是改善因传质限制而恶化的沸石催化剂性能的有效途径。