铈锆改性镍基催化剂制备及其甲烷三重整性能  

Preparation and performance of Ce,Zr-doped modified Ni-based catalysts for tri-reforming of CH_4

作　　者：薛茹君[1] 李丽[1] 王庆超[1] 

机构地区：[1]安徽理工大学化学工程学院,安徽淮南232001

出　　处：《合肥工业大学学报（自然科学版）》2014年第10期1173-1176,1280,共5页Journal of Hefei University of Technology：Natural Science

摘　　要：文章采用共沉淀法制得铈、锆掺杂氧化铝载体,以浸渍法负载活性组分镍得到Ni/CeO2-ZrO2-Al2O3催化剂,改善了CH4三重整反应的活性和稳定性。用EDS、XRD、BET、H2-TPR分别表征催化剂的组成、物相、比表面积和还原活性。考察了原料气组成n(CH4)∶n(CO2)∶n(H2O)∶n(O2)=1∶0.5∶0.5∶0.1时,催化剂在750℃、0.1MPa下对CH4三重整的稳定性及积碳性能。结果表明:ZrO2掺杂提高了催化剂的活性和稳定性;CeO2掺杂降低了Ni基催化剂的还原活化温度,且催化剂的稳定性更好;Al/Zr、Ce/Al的原子比分别为8和0.015的10%Ni/CeO2-ZrO2-Al2O3对CH4三重整的性能最好;反应100h后,催化剂的CH4转化率仍然大于87%,CO2转化率大于89%,积碳量仅为3.8%,催化剂的使用寿命大为延长。For the purpose of improving the activity and stability of the catalyst w hich w ould be used in the tri-reforming reaction of CH4 ,the active component Ni was impregnated on Ce ,Zr-doped Al2 O3 carrier prepared by co-precipitation .T he phase ,element composition ,specific surface area and reduc-ibility of the catalysts were characterized by means of XRD ,EDS ,BET and H2-TPR respectively . The stability and carbon deposition of the catalysts for the tri-reforming reaction of CH4 at 750 ℃ and 0.1 MPa were determined as the feed gas composition was n（CH4）∶ n（CO2）∶ n（H2O）∶ n（O2）=1∶0 .5∶0 .5∶0 .1 .The experimental results show that the catalytic activity and stability could be im-proved via compounding ZrO2 with Al2 O3 .The reduction-activating temperature of the catalyst could be further reduced via doping CeO2 into the ZrO2-Al2 O3 complex oxide ,and the stability of Ni/CeO2-ZrO2-Al2 O3 catalyst was better than that of Ni/ZrO2-Al2 O3 catalyst .Ni/CeO2-ZrO2-Al2 O3 catalyst with Ni mass fraction of 10% ,Al/Zr and Ce/Al atomic ratios of 8 and 0.015 respectively had better catalytic activity for tri-reforming reaction of CH4 .After having been used for 100 h at 750 ℃ and 0.1 MPa ,the CH4 conversion of the catalyst remained larger than 87% ,CO2 conversion of the cata-lyst remained larger than 89% ,and the amount of carbon deposit on the catalyst was only 3.8% . Thus the service life of the catalyst was greatly improved .

关 键 词：Ni/CeO2-ZrO2-Al2 O3 催化剂载体 改性 CH4 三自热重整 合成气 

分 类 号：O643[理学—物理化学] TQ426[理学—化学]