摘要
通过溶胶-凝胶方法制备了一系列不同Zn含量的Cu-Mn-Zn/ZrO_(2)催化剂,并通过XRD、BET、TPR、N_(2)O吸附、XPS、TPD和in-situ DRIFTS进行了表征。结果表明,随着Zn含量增加,催化剂上CO_(2)加氢反应的活性增加。在所有样品中,Cu_(3)MnZn_(0.5)Zr_(0.5)(CMZZ-0.5)在250℃和5 MPa条件下具有最高的CO_(2)转化率(6.5%)和甲醇选择性(73.7%)。表征结果表明,Zn进入Cu_(1.5)Mn_(1.5)O_(4)尖晶石结构,形成ZnOx,导致催化剂表面羟基含量的增加,同时增加了Cu0和Cu^(α+)的含量,改善了H_(2)和CO_(2)的活化能力。此外,通过原位漫反射红外光谱研究了CO_(2)转化为甲醇的途径。
A series of Cu-Mn-Zn/ZrO_(2)catalysts with different Zn contents were prepared by sol-gel method and characterized by XRD,BET,TPR,N2O-adsorption,XPS,TPD and in-situ DRIFTS.It was found that by increasing a certain amount of Zn,the catalytic activity for CO_(2)hydrogenation increased.Among all samples,Cu_(3)MnZn_(0.5)Zr_(0.5)(CMZZ-0.5)possessed the best CO_(2)conversion(6.5%)and methanol selectivity(73.7%)at 250°C and 5 MPa.Characterization results showed that Zn entered the Cu_(1.5)Mn_(1.5)O_(4) spinel structure,forming ZnOx and thus more surface OH groups.This increased the content of Cu0 and Cu^(α+),which improved the activation of H2 and CO_(2).The pathway of CO_(2)to methanol was also clarified through in-situ DRIFTS.
作者
王世威
杨金海
周宏利
肖福魁
赵宁
WANG Shiwei;YANG Jinhai;ZHOU Hongli;XIAO Fukui;ZHAO Ning(State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;University of Chinese Academy of Sciences,Beijing 100049,China)
出处
《燃料化学学报（中英文）》
EI
CAS
CSCD
北大核心
2024年第3期293-304,共12页
Journal of Fuel Chemistry and Technology
基金
supported by Fundamental Research Program of Shanxi Province(202203021221303)
Science and Technology Major Project of Shanxi Province(202005D121002)
The Central Project Guide Local Science and Technology for Development(2020SW26)。
