State Key Laboratory of Catalysis, 2011-Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
Science. 2023 May 19;380(6646):727-730. doi: 10.1126/science.adg2491. Epub 2023 May 18.
Breaking the trade-off between activity and selectivity has been a long-standing challenge in the field of catalysis. We demonstrate the importance of disentangling the target reaction from the secondary reactions for the case of direct syngas conversion to light olefins by incorporating germanium-substituted AlPO-18 within the framework of the metal oxide-zeolite (OXZEO) catalyst concept. The attenuated strength of the catalytically active Brønsted acid sites allows enhancing the targeted carbon-carbon coupling of ketene intermediates to form olefins by increasing the active site density while inhibiting secondary reactions that consume the olefins. Thus, a light-olefins selectivity of 83% among hydrocarbons and carbon monoxide conversion of 85% were obtained simultaneously, leading to an unprecedented light-olefins yield of 48% versus current reported light-olefins yields of ≤27%.
在催化领域,打破活性和选择性之间的权衡一直是一个长期存在的挑战。我们通过在金属氧化物-沸石(OXZEO)催化剂概念的框架内引入锗取代的 AlPO-18,证明了将目标反应与次级反应解耦的重要性,用于直接将合成气转化为低碳烯烃。催化活性的布朗斯台德酸位强度的减弱允许通过增加活性位密度来增强酮烯中间体的目标碳-碳偶联以形成烯烃,同时抑制消耗烯烃的次级反应。因此,在烃类和一氧化碳转化率为 85%的情况下,同时获得了 83%的低碳烯烃选择性,导致前所未有的低碳烯烃收率为 48%,而目前报道的低碳烯烃收率≤27%。