锌锆复合氧化物担载镍基催化剂用于甲烷干重整反应  

Zinc-zirconia composite oxide supported nickel catalysts for methane dry reforming reaction

作　　者：蔡国兵 储伟[1] 王佳杰[1] 施冰梅 CAI Guo-bing;CHU Wei;WANG Jia-jie;SHI Bing-mei(School of Chemical Engineering,Sichuan University,Chengdu 610065,China)

机构地区：[1]四川大学化学工程学院,四川成都610065

出　　处：《化学研究与应用》2023年第9期2205-2216,共12页Chemical Research and Application

摘　　要：采用一锅共沉淀法制备氧化锌改性的锌锆复合氧化物担载的镍基催化剂并用于甲烷二氧化碳干重整反应;研究了氧化锌含量对催化反应性能的影响,并通过XRD、H_(2)-TPR、CO_(2)-TPD、BET、XPS、SEM等手段分析了催化剂的理化性质和形貌。对比没有氧化锌助剂的氧化锆担载镍基对照样品,氧化锌的加入促进了活性组分Ni的分散和还原,增加了催化剂表面活性位Ni^(0)的含量,增加了催化剂的碱性位点的数量。优化的Ni/30%ZnO-ZrO_(2)催化剂表现出良好的催化活性,甲烷的表观活化能从没有氧化锌促进剂的63.5 kJ·mol^(-1)降低至43.4 kJ·mol^(-1),二氧化碳的表观活化能也从35.1 kJ·mol^(-1)降低至23.5 kJ·mol^(-1)。在50小时稳定性考察中只观察到细微的性能变化。A nickel-based catalyst supported on zinc-zirconium composite oxide modified with zinc oxide was prepared using a onepot co-precipitation method and applied in the dry reforming of methane with carbon dioxide.The effect of zinc oxide content on the catalytic performance was investigated,and the physicochemical properties and morphology of the catalyst were analyzed using various techniques such as XRD,H_(2)-TPR,CO_(2)-)TPD,BET,XPS,and SEM.Compared with the nickel catalyst supported on pure zirconia without zinc oxide additive,the addition of zinc oxide promoted the dispersion and reduction of the active component Ni,increased the content of Ni^(0) active sites on the catalyst surface,and increased the number of basic sites on the catalyst.The optimized Ni/30%Zn0-ZrO_(2) catalyst exhibited excellent catalytic activity,with the apparent activation energy of methane decreasing from 63.5 kJ·mol-^(1)for the catalyst without zinc oxide promoter to 43.4 kJ·mol^(-1),and the apparent activation energy of carbon dioxide decreasing from 35.1 kJ·mol^(-1) to 23.5 kJ·mol^(-1).Only slight performance changes were observed during the 50h stability test.

关 键 词：甲烷干重整 NI基催化剂 复合氧化物 ZnO促进剂 活化能 

分 类 号：O643.3[理学—物理化学]