Dynamic confinement of SAPO-17 cages on the selectivity control of syngas conversion  

作　　者：Haodi Wang Feng Jiao Yi Ding Wenjuan Liu Zhaochao Xu Xiulian Pan Xinhe Bao 

机构地区：[1]State Key Laboratory of Catalysis,2011-Collaborative Innovation Centerof Chemistry for Energy Materials,Dalian Institute of Chemical Physics,Chinese Academyof Sciences,Dalian 116023,China [2]Key Laboratory of Separation Science for Analytical Chemistry,Dalian Instituteof Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China [3]University of Chinese Academyof Sciences,Beijing 100049,China [4]Departmentof Chemical Physics,University of Science and Technology of China,Hefei 230026,China

出　　处：《National Science Review》2022年第9期35-41,共7页国家科学评论（英文版）

基　　金：supported by the Ministry of Science and Technology of China(2018YFA0704503);the National Natural Science Foundation of China(91945302 and22002153);the Youth Innovation Promotion Association of the Chinese Academy of Sciences(2019184);the Natural Science Foundation of Liaoning Province(2020-BS-019);the Dalian Science and Technology Innovation Fund(2020JJ26GX028)。

摘　　要：The OXZEO(oxide-zeolite)bifunctional catalyst concept has enabled selective syngas conversion to a series of value-added chemicals and fuels such as light olefins,aromatics and gasoline.Herein we report for the first time a dynamic confinement of SAPO-17 cages on the selectivity control of syngas conversion observed during an induction period.Structured illumination microscopy,intelligent gravimetric analysis,UV-Raman,X-ray diffraction,thermogravimetry and gas chromatography-mass spectrometer analysis indicate that this is attributed to the evolution of carbonaceous species as the reaction proceeds,which gradually reduces the effective space inside the cage.Consequently,the difusion of molecules is hindered and the hindering is much more prominent for larger molecules such as C_(4+).As a result,the selectivity of ethylene is enhanced whereas that of Cis suppressed.Beyond the induction period,the product selectivity levels off.For instance,ethylene selectivity levels off at 44%and propylene selectivity at 31%,as well as CO conversion at 27%.The findings here bring a new fundamental understanding that will guide further development of selective catalysts for olefin synthesis based on the OXZEO concept.

关 键 词：syngas conversion OXZEO dynamic confinement ZEOLITE DIFFUSION 

分 类 号：TQ221.2[化学工程—有机化工] TQ426