College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China.
Imaging and Characterization Department, KAUST Core Labs, King Abdullah University of Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia.
Angew Chem Int Ed Engl. 2023 Jun 12;62(24):e202303124. doi: 10.1002/anie.202303124. Epub 2023 May 3.
Decarbonizing the transportation sector is among the biggest challenges in the fight against climate change. CO -neutral fuels, such as those obtained from renewable methanol, have the potential to account for a large share of the solution, since these could be directly compatible with existing power trains. Although discovered in 1977, the zeolite-catalyzed methanol-to-gasoline (MTG) process has hardly reached industrial maturity, among other reasons, because maximizing the production of gasoline range hydrocarbons from methanol has proved complicated. In this work, we apply multimodal operando UV/Vis diffuse reflectance spectroscopy coupled with an online mass spectrometer and "mobility-dependent" solid-state NMR spectroscopy to better understand the reaction mechanism over zeolites H-Beta and Zn-Beta. Significantly, the influential co-catalytic role of oxymethylene species is linked to gasoline formation, which impacts the MTG process more than carbonylated species.
实现交通运输领域的脱碳是应对气候变化的最大挑战之一。CO 中性燃料,如可再生甲醇制成的燃料,有可能成为解决方案的重要组成部分,因为这些燃料可以直接与现有的动力传动系统兼容。尽管沸石催化甲醇制汽油(MTG)工艺早在 1977 年就已被发现,但它几乎没有达到工业化成熟阶段,其中一个原因是,从甲醇中最大化生产汽油范围的烃类化合物被证明很复杂。在这项工作中,我们应用多模态在位 UV/Vis 漫反射光谱结合在线质谱仪和“与迁移率相关”的固态 NMR 光谱来更好地理解沸石 H-Beta 和 Zn-Beta 上的反应机制。重要的是,亚甲氧基物种的协同催化作用与汽油的形成有关,这比羰基化物种对 MTG 过程的影响更大。