高硅ZSM-5沸石孔道和酸性的协同调控及其催化甲醇制丙烯反应性能  

A superior methanol-to-propylene catalyst:Construction via synergistic regulation of pore structure and acidic property of high-silica ZSM-5 zeolite

作　　者：李兴扬[1] 刘田菊 高阳 张丹丹 周勇 潘梦 LI Xingyang;LIU Tianju;GAO Yang;ZHANG Dandan;ZHOU Yong;PAN Meng(School of Chemical and Environmental Engineering,Anhui Polytechnic University,Wuhu,Anhui 241000,China;Eco-materials and Renewable Energy Research Center,School of Physics,Nanjing University,Nanjing 210000,China)

机构地区：[1]安徽工程大学化学与环境工程学院,芜湖241000 [2]南京大学物理学院,环境材料与再生能源研究中心,南京210000

出　　处：《无机化学学报》2024年第7期1279-1289,共11页Chinese Journal of Inorganic Chemistry

基　　金：国家自然科学基金(No.51572004);安徽省自然科学基金(No.2008085QB91);“洁净能源材料与资源物质转化化学”安徽省高校重点实验室开放基金(No.LCECSC-03);功能分子固体教育部重点实验室开放基金(No.FMS202007);安徽工程大学校级科研项目(No.Xjky2022106)资助。

摘　　要：通过碱处理结合铬改性策略实现了对高硅ZSM-5沸石孔道和酸性的协同调控,制备出了一种具有适宜酸性的高硅多级孔沸石催化剂。在碱处理的过程中,通过精细调节合成凝胶组成,在沸石晶体中引入的丰富共生界面,诱导了介孔的形成,从而打破了沸石硅铝比对常规碱处理法的限制。在铬改性的过程中,独特的多级孔结构促进了铬在催化剂中的分散,从而实现了对酸性的深度改性。在甲醇制丙烯催化反应中,制备的催化剂表现出了极佳的催化稳定性以及很高的丙烯和总低碳烯烃选择性。Combined strategy of alkali treatment and chromium modification was used to synergistically regulate the pore structure and acidic property of the high-silica ZSM-5 zeolite.During the alkaline treatment,the abundant intergrowth boundaries constructed by adjusting the composition of the synthesis gel induced the formation of mesopores.Thereby,the limitation of the conventional alkali treatment method coming from the framework Si/Al ratio of parent zeolite was circumvented.In the process of chromium modification,the unique hierarchical pore structure promoted the dispersion of chromium species in the catalyst.Thus,a deep modification of the acidic property was realized.As a result,a high-silica hierarchical zeolite catalyst with suitable acidities was obtained.During the catalytic conversion of methanol to propylene,the variation of the pore structure and acidic property caused obvious changes in the coke deposition behavior of the catalyst and the mass transfer of products.Consequently,the prepared catalyst exhibited excellent catalytic stability and a high selectivity towards propylene and total light olefins.

关 键 词：甲醇制丙烯 多级孔 酸性调控 沸石 催化性能 

分 类 号：O611.4[理学—无机化学]