Ristanović Zoran, Kerssens Marleen M, Kubarev Alexey V, Hendriks Frank C, Dedecker Peter, Hofkens Johan, Roeffaers Maarten B J, Weckhuysen Bert M
Debye Institute for Nanomaterials Science, Faculty of Science, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht (The Netherlands).
Angew Chem Int Ed Engl. 2015 Feb 2;54(6):1836-40. doi: 10.1002/anie.201410236. Epub 2014 Dec 12.
Fluid catalytic cracking (FCC) is a major process in oil refineries to produce gasoline and base chemicals from crude oil fractions. The spatial distribution and acidity of zeolite aggregates embedded within the 50-150 μm-sized FCC spheres heavily influence their catalytic performance. Single-molecule fluorescence-based imaging methods, namely nanometer accuracy by stochastic chemical reactions (NASCA) and super-resolution optical fluctuation imaging (SOFI) were used to study the catalytic activity of sub-micrometer zeolite ZSM-5 domains within real-life FCC catalyst particles. The formation of fluorescent product molecules taking place at Brønsted acid sites was monitored with single turnover sensitivity and high spatiotemporal resolution, providing detailed insight in dispersion and catalytic activity of zeolite ZSM-5 aggregates. The results point towards substantial differences in turnover frequencies between the zeolite aggregates, revealing significant intraparticle heterogeneities in Brønsted reactivity.
流化催化裂化(FCC)是炼油厂中从原油馏分生产汽油和基础化学品的主要工艺。嵌入50-150微米大小的FCC球体中的沸石聚集体的空间分布和酸度对其催化性能有重大影响。基于单分子荧光的成像方法,即通过随机化学反应实现纳米精度(NASCA)和超分辨率光学波动成像(SOFI),被用于研究实际FCC催化剂颗粒中亚微米级沸石ZSM-5区域的催化活性。在布朗斯台德酸位点发生的荧光产物分子的形成以单周转灵敏度和高时空分辨率进行监测,从而深入了解沸石ZSM-5聚集体的分散性和催化活性。结果表明沸石聚集体之间的周转频率存在显著差异,揭示了布朗斯台德反应性在颗粒内存在显著的不均匀性。