Cu-Ni-Al尖晶石催化甲醇水蒸气重整制氢性能的研究  

Catalytic performance of Cu-Ni-Al spinel for methanol steam reforming to hydrogen

作　　者：庆绍军[1,2] 侯晓宁 刘雅杰[1] 王磊 李林东[1] 高志贤[1] QING Shao-jun;HOU Xiao-ning;LIU Ya-jie;WANG Lei;LI Lin-dong;GAO Zhi-xian(Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;University of Chinese Academy of Sciences,Beijing 100049,China;School of Chemistry and Chemical Engineering,Xinjiang University,Urumqi 830046,China)

机构地区：[1]中国科学院山西煤炭化学研究所,山西太原030001 [2]中国科学院大学,北京100049 [3]新疆大学化学化工学院,新疆乌鲁木齐830046

出　　处：《燃料化学学报》2018年第10期1210-1217,共8页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21503254;21673270;21763018)资助~~

摘　　要：以氢氧化铜、醋酸镍和拟薄水铝石为原料,通过固相法合成了Cu-Ni-Al尖晶石催化剂。采用N2物理吸附、XRD、H2-TPR和XPS等表征方法,研究Cu/Ni/Al的物质的量比和焙烧温度对催化剂的比表面积、物相、还原性能以及表面性质的影响,并以甲醇水蒸气重整制氢为探针反应,考察催化剂的缓释催化性能。结果表明,随着焙烧温度的升高,Cu-Ni-Al催化剂的尖晶石含量增加,但尖晶石晶粒增大,且比表面积下降。不同的焙烧温度和Cu/Ni/Al物质的量比,所得催化剂的比表面积、还原性能和表面性质不同,从而表现出不同的缓释催化性能。与计量比Cu/Al=1∶2的合成比较,Cu/Al=1∶3形成了非计量比的富Al尖晶石固溶体,生成的晶体粒子小、比表面积和孔容大、难还原的尖晶石部分增多,呈现出更好的缓释催化性能。甲醇制氢反应性能评价结果显示,Cu-Ni-Al尖晶石在反应条件下逐渐释放活性铜而催化反应的进行,其中,CNA3-1000催化剂表现中最高的催化活性和稳定性。Using copper hydroxide,nickel acetate and pseudoboehmite as materials,the Cu-Ni-Al spinel catalysts were synthesized by the solid-phase method.The effects of Cu/Ni/Al molar ratio and calcination temperature on specific surface area,phase composition,reduction performance and surface property of Cu-Ni-Al spinel catalysts were characterized by BET,XRD,H 2-TPR and XPS.Moreover,the sustained release catalytic performances of Cu-Ni-Al spinel samples for methanol steam reforming were tested.The obtained results indicated that with increasing the calcination temperature,the content of Cu-Ni-Al spinel increased,but the size of spinel particles increased and the specific surface area decreased.Change of the calcination temperature and Cu/Ni/Al molar ratio led to different specific surface area,reduction performance and surface property of Cu-Ni-Al spinel catalysts,thus showing different sustained release catalytic performance.Comparing with those of stoichiometric ratio of Cu/Al=1∶2,spinel solid solutions with smaller particle size,higher specific surface area and pore volume,more hardly-reducible spinel and better sustained release catalytic performance were obtained with the nonstoichiometric ratio of Cu/Al=1∶3.The results of catalyst evaluation indicated that active copper species were released from Cu-Ni-Al spinel lattice and thus took part in the catalytic action.Among the prepared catalysts,CNA3-1000 catalyst showed the highest catalytic activity and stability.

关 键 词：Cu-Ni-Al尖晶石 固相法 甲醇重整 氢气 

分 类 号：O643.322[理学—物理化学]