Zr对CuO/ZnO/Al_2O_3前驱体物相、催化剂结构及其合成甲醇性能的影响  

Effect of Zr on CuO/ZnO/Al_2O_3 Precursor Composition,Structure and Catalysis for Methanol Synthesis

作　　者：李忠[1] 刘岩[1] 范辉[1] 郑华艳[1] 

机构地区：[1]太原理工大学煤化工研究所,煤科学与技术教育部和山西省重点实验室,太原030024

出　　处：《无机化学学报》2010年第7期1245-1251,共7页Chinese Journal of Inorganic Chemistry

基　　金：国家重点基础研究发展计划(973计划,No.2005CB221204)资助项目

摘　　要：采用并流共沉淀法,在CuO/ZnO/Al2O3三元催化剂中加入第四组分Zr,考察了沉淀温度对四元催化剂的前驱体物相组成及浆态床合成甲醇催化活性的影响。通过XRD、DTG、TPR、FTIR、CO-TPD、XPS、HR-TEM等对所制备催化剂及其前驱体的微观结构进行了表征。研究表明:Zr促进了绿铜锌矿(Cu,Zn)5(CO3)2(OH)6物相的生成,使催化剂前驱体中绿铜锌矿含量增加,焙烧后的催化剂铜锌协同作用增强,CuO分散度提高,CuO晶粒平均直径只有4.18nm,同时还原温度显著降低为150℃,CO吸附能力增强,结果显著提高了浆态床合成甲醇催化活性和稳定性。与CuO/ZnO/Al2O3三元催化剂相比,80℃沉淀制备的含4%Zr的CuO/ZnO/Al2O3/ZrO2四元催化剂的甲醇时空收率提高了8.67%,失活率降低了65.12%。Zr was introduced in the preparation of CuO/ZnO/Al2O3 catalyst precursor by co-precipitation.The precursors composition,catalyst structure and catalytic activity were investigated at the precipitation temperature.The precursors and catalysts were characterized by XRD,DTG,TPR,FTIR,XPS,HR-TEM and CO-TPD.The results show that the precursor with Zr has more（Cu,Zn）5（CO3）2（OH）6 phase.The calcined catalyst with Zr has better CuOZnO synergy,smaller CuO crystal particle,more adsorption ability of CO and lower reduction temperature,resulting in better activity and stability for slurry methanol synthesis.In contrast to CuO/ZnO/Al2O3 catalyst,the CuO/ZnO/Al2O3/ZrO2 catalyst precipitated at 80 ℃ exhibits that space time yield（STY） raises by 8.67% and deactivation rate declines by 65.12%.

关 键 词：甲醇 CuO/ZnO/Al2O3/ZrO2 浆态床 共沉淀 

分 类 号：O614.121[理学—无机化学] O614.24[理学—化学]