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Disentangling the activity-selectivity trade-off in catalytic conversion of syngas to light olefins
Science ( IF 44.7 ) Pub Date : 2023-05-18 , DOI: 10.1126/science.adg2491
Feng Jiao 1, 2 , Bing Bai 1, 2 , Gen Li 1, 2 , Xiulian Pan 1, 2 , Yihan Ye 1, 2 , Shengcheng Qu 1 , Changqi Xu 1 , Jianping Xiao 1, 2 , Zhenghao Jia 1 , Wei Liu 1 , Tao Peng 1, 3 , Yilun Ding 1, 2 , Cheng Liu 1, 2 , Jinjing Li 1 , Xinhe Bao 1, 2, 3
Affiliation  

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%.

中文翻译:

解开合成气催化转化为轻烯烃的活性-选择性权衡

打破活性和选择性之间的权衡一直是催化领域的一个长期挑战。我们证明了通过在金属氧化物-沸石 (OXZEO) 催化剂概念的框架内结合锗取代的 AlPO-18,将目标反应与次级反应分开对于直接合成气转化为轻质烯烃的重要性。催化活性 Brønsted 酸位点的衰减强度允许通过增加活性位点密度同时抑制消耗烯烃的二次反应来增强乙烯酮中间体的目标碳-碳偶联以形成烯烃。因此,同时获得83%的烃类轻烯烃选择性和85%的一氧化碳转化率,
更新日期:2023-05-18
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