Direct propylene epoxidation with molecular oxygen over titanosilicate zeolites  

作　　者：Weijie Li Bin Qin Zhuoya Dong Yuchao Chai Guangjun Wu Yanhang Ma Meng Wang Xingwu Liu Ding Ma Landong Li 

机构地区：[1]Key Laboratory of Advanced Energy Materials Chemistry of Ministry of Education,College of Chemistry,Nankai University,Tianjin 300071,China [2]School of Physical Science and Technology,ShanghaiTech University,Shanghai 201210,China [3]Beijing National Laboratory for Molecular Sciences,New Cornerstone Science Laboratory,College of Chemistry and Molecular Engineering,Peking University,Beijing 100871,China [4]Frontiers Science Center for New Organic Matter,College of Chemistry,Nankai University,Tianjin 300071,China

出　　处：《National Science Review》2024年第11期133-141,共9页国家科学评论（英文版）

基　　金：supported by the National Natural Science Foundation of China(22025203 and 22121005);the National Key R&D Program of China(2021YFA1501102);Haihe Laboratory of Sustainable Chemical Transformations,Tianjin.D.M.acknowledges support from the Tencent Foundation through the XPLORER PRIZE.

摘　　要：The direct epoxidation of propylene with molecular oxygen represents a desired route for propylene oxide(PO)production with 100%theoretical atomic economy.However,this aerobic epoxidation reaction suffers from the apparent trade-off between propylene conversion and PO selectivity,and remains a key challenge in catalysis.We report that Ti-Beta zeolites containing isolated framework Ti species can efficiently catalyze the aerobic epoxidation of propylene.Stable propylene conversion of 25%and PO selectivity of up to 90%are achieved at the same time,matching the levels of industrial ethylene aerobic epoxidation processes.H-terminated pentacoordinated Ti species in Beta zeolite frameworks are identified as the preferred active sites for propylene aerobic epoxidation and the reaction is initiated by the participation of lattice oxygen in Ti-OH.These results are expected to spark new technology for the industrial production of PO toward more sustainable chemistry and chemical engineering.

关 键 词：titanosilicate zeolites propylene epoxidation molecular oxygen 

分 类 号：TQ426[化学工程]