Co/Ce_xTi_(1-x)O_2催化剂的制备及其对甲烷部分氧化反应催化性能  

Preparation of Co/Ce_xTi_(1-x)O_2 Catalysts and Their Catalytic Performance in Partial Oxidation of Methane

作　　者：余长林[1] 周晓春[1] 胡久彪[1] 相彬[2] 陈建钗[1] 魏龙福[1] 

机构地区：[1]江西理工大学冶金与化学工程学院,江西赣州341000 [2]大连理工大学附属高中,辽宁大连116024

出　　处：《石油学报（石油加工）》2013年第6期966-974,共9页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金(21067004;21263005);江西省教育厅科技基金(GJJ12344);江西省青年科学家培养项目(20122BCB23015)资助

摘　　要：采用柠檬酸络合法制备了Cex Ti1-x O2固溶体,以其为载体浸渍硝酸钴溶液制备负载钴催化剂mCo/Cex Ti1-x O2-T-y。考察了Co负载量(m)、载体中Ce/(Ce+Ti)摩尔比(x)、载体制备过程中柠檬酸用量(y)以及载体的焙烧温度(T)对该系列催化剂催化甲烷部分氧化(POM)制合成气反应性能的影响。利用X射线粉末衍射(XRD)、H2-程序升温还原(H2-TPR)、扫描电子显微镜(SEM)和热重(TG)分析手段对mCo/Cex Ti1-x O2-T-y催化剂进行了表征。结果表明,当负载Co的质量分数为20%、柠檬酸/(Ce+Ti)的摩尔比为1、载体焙烧温度为700℃时,制备的20Co/Ce0.5Ti0.5O2-700-1催化剂对POM反应表现出优良的催化性能,其主要原因是,载体之间形成的Ce-Ti固溶体能够一定程度上抑制非催化活性相CoTiO3的生成。A series of CexTi1-xO2 solid solutions were prepared by citric acid complex method. Then the as-synthesized CexTi1-xO2 solid solutions were used as the supports and Co with different contents were loaded by impregnating method, producing Co supported mCo/CexTi1-xO2-T-y catalysts. The effects of Co content （m）, Ce/（Ce＋Ti） molar ratio in support（x）, the used amount of citric acid（y）, and the calcination temperature （T） on the catalytic performance of mCo/CexTi1-xO2-T-y in partial oxidation of methane （POM） to synthesis gas were investigated. Some techniques, such as X-ray diffraction（XRD）, temperature programmed reduction（TPR） of H2, scanning electron microscopy（SEM） and thermogravimetry analysis （TG） were used to characterize the fresh and reacted catalysts. The results showed that the catalyst（20Co/Ce0.5Ti0.5O2-700-1） with Co loading of 20%, the citric/（Ce＋Ti） molar ratio of 1 and the support calcination temperature of 700℃ exhibited the excellent catalytic performance in POM reaction. The high catalytic performance could be attributed to that the formation of Ce＋Ti solid solution could effectively restrain the generation of non-active component of CoTiO3.

关 键 词：CO CexTi1-x O2固溶体 钴 甲烷部分氧化 钛酸钴 载体 

分 类 号：TQ032[化学工程] O643[理学—物理化学]