铈源对甲醇水蒸气重整制氢CuO/CeO2催化剂的影响  

Influence of cerium sources on CuO/CeO catalysts for hydrogen production from steam reforming of methanol

作　　者：王丽宝 王东哲 张磊[1] 庆绍军[2] 韩蛟 张财顺 高志贤 张海娟[1] 冯旭浩 WANG Li-bao;WANG Dong-zhe;ZHANG Lei;QING Shao-jun;HAN Jiao;ZHANG Cai-shun;GAO Zhi-xian;ZHANG Hai-juan;FENG Xu-hao(Petrochemical College,Liaoning Shihua University,Fushun 113001,China;Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;No.3 Refinery of Fushun Petrochemical Company,CNPC,Fushun 113001,China)

机构地区：[1]辽宁石油化工大学石油化工学院,辽宁抚顺113001 [2]中国科学院山西煤炭化学研究所,山西太原030001 [3]中国石油天然气股份有限公司抚顺石化分公司石油三厂,辽宁抚顺113001

出　　处：《燃料化学学报》2020年第7期852-859,共8页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21376237);辽宁省教育厅科学研究经费项目(L2019038);辽宁省自然科学基金(2019-MS-221)资助。

摘　　要：采用沉淀法合成了CeO2载体,再经浸渍法负载活性组分得到CuO/CeO2催化材料,探究了铈源(Ce(NO3)3·6H2O、Ce Cl3·6H2O、Ce(NH4)2(NO3)6、Ce(SO4)2·4H2O)对CuO/CeO2催化性能的影响。通过采用XRD、SEM、N2O滴定、BET和H2-TPR等表征手段对催化材料的结构和性质研究发现,四种铈源合成的CuO/CeO2催化材料在Cu比表面积、还原性能以及活性组分和载体间的相互作用方面存在着明显差别。其中,由Ce(NO3)3·6H2O合成的CuO/CeO2催化材料的Cu比表面积较大,CuO还原温度较低,CeO2载体与CuO之间相互作用较强,在甲醇水蒸气重整反应过程中,表现出较佳的催化活性,在反应温度为553 K,水醇比n(H2O)/n(MeOH)为1.2,甲醇水蒸气气体空速(GHSV)为1760 h-1时,甲醇的转化率为100%,重整气中CO摩尔含量为0.84%。CeO2 support was synthesized by precipitation method and used to prepare CuO/CeO2 catalyst using impregnation method.The effects of cerium sources(Ce(NO3)3·6 H2 O,CeCl3·6 H2 O,Ce(NH4)2(NO3)6 and Ce(SO4)2·4 H2 O) on the catalytic performance of CuO/CeO2 catalyst were investigated.XRD,SEM, N2 O titration,BET and H2-TPR were used to study the structure and properties of the catalysts.The CuO/CeO2 catalysts with different cerium sources have obvious differences in Cu specific surface area,reduction performance and interaction between active component and support.Moreover,CuO/CeO2 catalyst prepared with Ce(NO3)3·6 H2 O has large Cu specific surface area,low reduction temperature and strong interaction between CeO2 support and CuO and shows better catalytic activity in methanol steam reforming.The methanol conversion is 100% at reaction temperature of 553 K,water/methanol ratio in feed of 1.2 and methanol water gas hourly space velocity of 1760 h-1.Besides,the CO molar content in reformed gas is 0.84%.

关 键 词：沉淀法 铈源 甲醇水蒸气重整 氢气 

分 类 号：O643[理学—物理化学]