Disentangling the activity-selectivity trade-off in catalytic conversion of syngas to light olefins

• 成果类型: Article
• 署名作者: Jiao, Feng; Bai, Bing; Li, Gen; Pan, Xiulian; Ye, Yihan; Qu, Shengcheng; Xu, Changqi; Xiao, Jianping; Jia, Zhenghao; Liu, Wei; Peng, Tao; Ding, Yilun; Liu, Cheng; Li, Jinjing; Bao, Xinhe
• 署名单位: Chinese Academy of Sciences; Dalian Institute of Chemical Physics, CAS; Chinese Academy of Sciences; University of Chinese Academy of Sciences, CAS; Chinese Academy of Sciences; University of Science & Technology of China, CAS
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-8226
• DOI: 10.1126/science.adg2491
• 发表日期: 2023-05-19
• 页码: 727-730
• 关键词: synthesis gas; hydrogenation; DESIGN; sites

摘要

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-1 8 within the framework of the metal oxide-zeolite (OXZEO) catalyst concept. The attenuated strength of the catalytically active Bronsted 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%.