燃料化学学报（中英文）2025，Vol.53Issue(7)：1038-1049,12.DOI:10.1016/S1872-5813(25)60535-4
改性ZnZrOx耦合ZSM-5催化CO2加氢制芳烃
Modified ZnZrOx coupled with ZSM-5 as the catalyst for the hydrogenation of CO2 to aromatics
摘要
Abstract
Direct hydrogenation of CO2 to aromatics via the methanol-mediated route over an oxide-zeolite bifunctional catalyst has received considerable attention in recent years.However,the activation of CO2 at mild condition remains a great challenge,as it needs to conquer a high activation energy barrier due to the chemical inertness of CO2.Herein,ZnZrOx oxides were modified by a series of transition metals(M=Fe,Cu,Co,Ni)and the modified M-ZnZrOx oxides were further used together with the commercial ZSM-5 zeolite to comprise the bifunctional M-ZnZrOx/ZSM-5 composite catalysts for the direct hydrogenation of CO2 to aromatics.The results indicate that the iron-modified Fe-ZnZrOx/ZSM-5 catalysts have abundant oxygen vacancies which are active for the transformation CO2 to aromatics;under 275 ℃,H2/CO2=3,and a space velocity of 600 mL/(gh),the Fe(4)-ZnZrOx/ZSM-5 catalyst with an Fe mass fraction of 4％achieves a selectivity of 80.4％to aromatics,where tetramethylbenzene accounts for more than 70.4％,with a single-pass CO2 conversion of 5.6％.A further increase of the Fe content to 8％can even improve the selectivity to aromatics(85.0％).Such observation should be useful for the design of industrial catalysts efficient for the direct conversion of CO2 to aromatics.关键词
二氧化碳加氢/芳烃/复合催化剂/ZnZrOx/金属改性Key words
carbon dioxide hydrogenation/aromatics/composite catalyst/ZnZrOx/metal modification分类
化学化工引用本文复制引用
秘亚鹏,于幸,卜宪昵,孙予罕,高鹏..改性ZnZrOx耦合ZSM-5催化CO2加氢制芳烃[J].燃料化学学报（中英文）,2025,53(7):1038-1049,12.基金项目
The project was supported by the National Natural Science Foundation of China(22293023,22172189,22293025),CAS Youth Interdisciplinary Team,Program of Shanghai Academic Research Leader(22XD1424100),Shanghai Municipal Science and Technology Commission,China(23ZR1481700)and Talent Plan of Shanghai Branch,Chinese Academy of Sciences(C ASSHB-QNPD-2023-024).国家自然科学基金(22293023,22172189,22293025),中国科学院青年交叉团队,上海市优秀学术带头人计划(22XD1424100),上海市自然科学基金(23ZR1481700)和中国科学院上海分院青年攀登计划(CASSHB-QNPD-2023-024)资助 （22293023,22172189,22293025）
