Zr改性Ni/γ-Al_2O_3催化剂用于浆态相合成气的低温甲烷化  

Low temperature methanation of syngas in a slurry reactor over Zr-doped Ni/γ-Al_2O_3 catalyst

作　　者：张俊峰[1] 白云星[1,2] 张清德[1] 解红娟[1] 谭猗生[1] 韩怡卓[1] 

机构地区：[1]中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001 [2]中国科学院大学,北京100049

出　　处：《燃料化学学报》2013年第8期966-971,共6页Journal of Fuel Chemistry and Technology

基　　金：国际合作项目-荷兰壳牌公司合作项目

摘　　要：采用浆态床反应器,在低温(300～330℃)下进行合成气的甲烷化反应。实验中通过共浸渍法(包括含浸-旋蒸法)制备了锆(Zr)修饰的Ni/γ-Al2O3催化剂,并考察其与单一NiO、未掺杂Zr的Ni/γ-Al2O3催化剂的催化性能差异。研究表明,载体γ-Al2O3的引入能够明显地提高CO的转化率和甲烷的选择性,而Zr的掺杂会进一步提升催化剂的催化活性。在325℃,空速为4 200 mL.g-1.h-1时,CO的转化率可以达到86.41%,甲烷选择性为90.53%。催化剂的表征结果表明,Zr的添加促进了Ni在催化剂表面的分散、减弱了活性Ni与载体的相互作用,抑制了低甲烷化活性的NiAl2O4的生成,使得催化剂的反应性能得到较大提高。Zr-doped Ni/γ-Al2O3 catalyst was prepared by co-impregnation of Ni and Zr on γ-Al2O3 ; over it, the methanation of syngas at low temperature （300 - 330 ℃ ） in a slurry reactor was investigated, Compared with single NiO and Ni/γ-Al2O3, the catalytic performance of the Zr-doped Ni/γ-Al2O3 is greatly improved. Under optimized condition, a high CO conversion of 86.41% and a selectivity of 90.53% to CH4 are achieved at a GHSV of 4 200 mL. g-1 .h-1. XRD, TEM and H2-TPR results suggest that the doping of Zr promotes dispersion of Ni on γ-Al2O3, weakens the interaction between Ni and the support and suppresses the formation of NiAl2O4 spinel with low methanation activity; all these may contribute to the excellent performance of the Zr-doped Ni/γ-Al2O3 catalyst in syngas methanation.

关 键 词：合成气 甲烷化 天然气 浆态床 低温 

分 类 号：O643[理学—物理化学]