The influence of intimacy on the ’iterative reactions’ during OX-ZEO process for aromatic production  

作　　者：Xiaoli Yang Ting Sun Junguo Ma Xiong Su Ruifeng Wang Yaru Zhang Hongmin Duan Yanqiang Huang Tao Zhang 

机构地区：[1]State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences,Dalian 116023, Liaoning, China [2]University of Chinese Academy of Sciences,Beijing 100049,China [3]College of Chemistry and Materials Science, Sichuan Normal University,Chengdu 610068, Sichuan, China

出　　处：《Journal of Energy Chemistry》2019年第8期60-65,I0003,共7页能源化学（英文版）

基　　金：the National Key R&D Program of China(2016YFA0202804);the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020400);the National Natural Science Foundation of China(Nos.21506204,21476226);Dalian Science Foundation for Distinguished Young Scholars(2016RJ04);the Youth Innovation Promotion Association CAS for financial support

摘　　要：The oxide-zeolite process provides a promising way for one-step production of aromatics from syngas,whereas the reasons for the dramatic effect of intimacy between oxide and zeolite in the composite catalyst on the product selectivity are still unclear. In order to explore the optimal intimacy and the essential influence factors, ZnCrOxcombined with ZSM-5 are employed to prepare the composite catalysts with different distances between the two components by changing the mixing methods. An aromatic selectivity of 74%(with CO conversion to be 16%) is achieved by the composite catalyst when the intimacy is in the range of nanometer. A so-called ‘iterative reactions’ mechanism of intermediates over oxides is then proposed and studied: the intermediate chemical can undergo a hydrogenation reaction on oxide.So the shorter the intermediates stay on oxide, the more of chance for C-C coupling takes place on zeolite to form aromatics. Moreover, the aero-environments of reaction is found to impact on the extent of iterative reaction as well. Therefore, when the intimacy between the two components changes, the extent of iterative reactions vary, resulting in alteration of product distribution. This work provides new insight in understanding the mechanisms during the complex process of OX-ZEO composite catalysis and sheds light to the design of a high-yield catalyst for synthetization of aromatics from syngas.The oxide-zeolite process provides a promising way for one-step production of aromatics from syngas,whereas the reasons for the dramatic effect of intimacy between oxide and zeolite in the composite catalyst on the product selectivity are still unclear. In order to explore the optimal intimacy and the essential influence factors, ZnCrOxcombined with ZSM-5 are employed to prepare the composite catalysts with different distances between the two components by changing the mixing methods. An aromatic selectivity of 74%(with CO conversion to be 16%) is achieved by the composite catalyst when the intimacy is in the range of nanometer. A so-called ‘iterative reactions’ mechanism of intermediates over oxides is then proposed and studied: the intermediate chemical can undergo a hydrogenation reaction on oxide.So the shorter the intermediates stay on oxide, the more of chance for C-C coupling takes place on zeolite to form aromatics. Moreover, the aero-environments of reaction is found to impact on the extent of iterative reaction as well. Therefore, when the intimacy between the two components changes, the extent of iterative reactions vary, resulting in alteration of product distribution. This work provides new insight in understanding the mechanisms during the complex process of OX-ZEO composite catalysis and sheds light to the design of a high-yield catalyst for synthetization of aromatics from syngas.

关 键 词：OX-ZEO PROCESS INTIMACY ITERATIVE REACTIONS Reaction aero-environment Diffusion 

分 类 号：TQ426[化学工程] TQ241