Cu/ZnO催化剂的金属载体相互作用及其对糠醛加氢制糠醇反应性能的影响  

Effect of the metal-support interaction in the Cu/ZnO catalyst on its performance in the hydrogenation of furfural to furfuryl alcohol

作　　者：于欣瑞 张金玉 杨海兴 种思颖 刘蝈蝈 张雅静 王康军 YU Xinrui;ZHANG Jinyu;YANG Haixing;CHONG Siying;LIU Guoguo;ZHANG Yajing;WANG Kangjun(College of Chemical Engineering,Shenyang University of Chemical Technology,Shenyang 110142,China)

机构地区：[1]沈阳化工大学化学工程学院,辽宁沈阳110142

出　　处：《燃料化学学报（中英文）》2024年第8期1045-1056,共12页Journal of Fuel Chemistry and Technology

基　　金：辽宁省高等学校创新人才支持计划(辽教函[2020]389号);辽宁省教育厅项目(LJKQZ20222266);沈阳市中青年科技创新人才支持计划(RC210365);辽宁省科技厅联合基金(2023-BSBA-276);达标立项项目(LDB2022001)资助。

摘　　要：采用共沉淀法制备了系列Cu/Zn比不同的Cu/ZnO催化剂,研究了Cu/Zn比与金属载体强相互作用(SMSI)的关系及其对糠醛气相加氢制糠醇催化反应性能的影响。XRD、H2-TPR、SEM、HRTEM和XPS等表征结果显示,Cu/ZnO催化剂中的金属载体强相互作用改变了催化剂的微观结构。ZnO载体对活性金属Cu颗粒具有不同程度的几何修饰,影响了Cu表面的电子状态。不同Cu/Zn比的Cu/ZnO催化剂的SMSI作用顺序为:20Cu/ZnO>40Cu/ZnO>60Cu/ZnO>80Cu/ZnO。在同一反应条件下,20Cu/ZnO催化剂的糠醛转化率高于80%的时间仅为5 h,而60Cu/ZnO催化剂的糠醛转化率高于80%的时间可以达到28 h,表明适当的SMSI作用有利于提升Cu/ZnO催化剂在糠醛加氢反应中的稳定性,而过强的SMSI作用会抑制其催化活性。A series of Cu/ZnO catalysts were prepared by the coprecipitation method and the effect of Cu/Zn ratio on the strong metal support interaction(SMSI)as well as its relation to the catalytic performance of Cu/ZnO in the gaseous hydrogenation of furfural to furfuryl alcohol was investigated.The H2-TPR,XRD,SEM,TEM and XPS characterization results reveal that there exists the SMSI effect in the Cu/ZnO catalyst that influences the catalyst microstructure.ZnO support,acting as a geometric modifier on the active metal Cu particles,has a significant influence on the electronic state of the surface Cu species.The strength of SMSI is related to the Cu/Zn ratio and the SMSI strength of various Cu/ZnO catalysts follows the order of 20Cu/ZnO>40Cu/ZnO>60Cu/ZnO>80Cu/ZnO.Under the same reaction conditions,the lifetime of the 20Cu/ZnO catalyst with a furfural conversion of above 80%is only 5 h,in comparison with the lifetime of 28 h for the 60Cu/ZnO catalyst.That is,appropriate SMSI can enhance the stability of the Cu/ZnO catalyst in the hydrogenation of furfural to furfuryl alcohol,whereas excessive SMSI is detrimental to the catalyst activity.

关 键 词：Cu/ZnO催化剂 金属载体强相互作用 几何修饰作用 糠醛加氢 糠醇 

分 类 号：TQ426.8[化学工程]