Zn含量对于Cu-Mn-Zn/ZrO_(2)催化剂CO_(2)加氢合成甲醇性能的影响研究  

Performance of Cu-Mn-Zn/ZrO_(2)catalysts for methanol synthesis from CO_(2)hydrogenation:The effect of Zn content

作　　者：王世威 杨金海[1] 周宏利 肖福魁[1] 赵宁[1] 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)

机构地区：[1]中国科学院山西煤炭化学研究所煤炭高效低碳转化全国重点实验室,山西太原030001 [2]中国科学院大学,北京100049

出　　处：《燃料化学学报（中英文）》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)。

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.

关 键 词：CO_(2)加氢 甲醇 Cu-基催化剂 表面羟基 

分 类 号：O643[理学—物理化学]