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Dr. Donglong Fu Onno van der Heijden Katarina Stanciakova Dr. Joel E. Schmidt Prof. Dr. Bert M. Weckhuysen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(36):15632-15636
Establishing structure–reactivity relationships for specific channel orientations of zeolites is vital to developing new, superior materials for various applications, including oil and gas conversion processes. Herein, a well-defined model system was developed to build structure–reactivity relationships for specific zeolite-channel orientations during various catalytic reaction processes, for example, the methanol- and ethanol-to-hydrocarbons (MTH and ETH) process as well as oligomerization reactions. The entrapped and effluent hydrocarbons from single-oriented zeolite ZSM-5 channels during the MTH process were monitored by using operando UV/Vis diffuse reflectance spectroscopy (DRS) and on-line mass spectrometry (MS), respectively. The results reveal that the straight channels favor the formation of internal coke, promoting the aromatic cycle. Furthermore, the sinusoidal channels produce aromatics, (e.g., toluene) that further grow into larger polyaromatics (e.g., graphitic coke) leading to deactivation of the zeolites. This underscores the importance of careful engineering of materials to suppress coke formation and tune product distribution by rational control of the location of zeolite acid sites and crystallographic orientations. 相似文献
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Gerardo Algara‐Siller Nikolai Severin Samantha Y. Chong Torbjrn Bjrkman Robert G. Palgrave Andrea Laybourn Markus Antonietti Yaroslav Z. Khimyak Arkady V. Krasheninnikov Jürgen P. Rabe Ute Kaiser Andrew I. Cooper Arne Thomas Michael J. Bojdys 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2014,126(29)
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