Wang Yuhao, Wang Genyuan, van der Wal Lars I, Cheng Kang, Zhang Qinghong, de Jong Krijn P, Wang Ye
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, 3584 CG, Utrecht, The Netherlands.
Angew Chem Int Ed Engl. 2021 Aug 2;60(32):17735-17743. doi: 10.1002/anie.202107264. Epub 2021 Jun 30.
The catalytic performance of composite catalysts is not only affected by the physicochemical properties of each component, but also the proximity and interaction between them. Herein, we employ four representative oxides (In O , ZnO, Cr O , and ZrO ) to combine with H-ZSM-5 for the hydrogenation of CO to hydrocarbons directed by methanol intermediate and clarify the correlation between metal migration and the catalytic performance. The migration of metals to zeolite driven by the harsh reaction conditions can be visualized by electron microscopy, meanwhile, the change of zeolite acidity is also carefully characterized. The protonic sites of H-ZSM-5 are neutralized by mobile indium and zinc species via a solid ion-exchange mechanism, resulting in a drastic decrease of C hydrocarbon products over In O /H-ZSM-5 and ZnO/H-ZSM-5. While, the thermomigration ability of chromium and zirconium species is not significant, endowing Cr O /H-ZSM-5 and ZrO /H-ZSM-5 catalysts with high selectivity of C hydrocarbons.
复合催化剂的催化性能不仅受各组分物理化学性质的影响，还受它们之间的距离和相互作用的影响。在此，我们采用四种代表性氧化物（In₂O₃、ZnO、Cr₂O₃和ZrO₂）与H-ZSM-5结合，用于由甲醇中间体导向的CO加氢制烃反应，并阐明金属迁移与催化性能之间的相关性。通过电子显微镜可以观察到在苛刻反应条件下金属向沸石的迁移，同时，也对沸石酸度的变化进行了仔细表征。H-ZSM-5的质子位点通过固体离子交换机制被移动的铟和锌物种中和，导致In₂O₃/H-ZSM-5和ZnO/H-ZSM-5上C₂烃产物急剧减少。而铬和锆物种的热迁移能力不显著，使Cr₂O₃/H-ZSM-5和ZrO₂/H-ZSM-5催化剂具有高的C₂烃选择性。
