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作 者:薛青松[1] 高立达[1] 路勇[1] 何鸣元[1]
机构地区:[1]华东师范大学化学系上海市绿色化学与化工过程绿色化重点实验室,上海200062
出 处:《石油化工》2008年第9期878-882,共5页Petrochemical Technology
基 金:国家自然科学基金项目(20590366;20573036);"863"计划项目(2007AA05Z101);新世纪优秀人才支持计划项目(06-NCET-0423);上海市"曙光计划"项目(06SG28);上海市重点学科建设项目(B409);华东师范大学2008年优秀博士研究生培养基金资助项目(20080013)
摘 要:以硫含量为500 μg/g 的零售汽油为原料,考察了水与碳的摩尔比、O_2与碳的摩尔比、反应温度和汽油重时空速对 Pt/CeO_2/Al_2O_3催化剂自热重整性能的影响,得到了优化的反应条件,并在优化条件下考察了 Pt/CeO_2Al_2O_3催化剂自热重整高含硫汽油的稳定性。实验结果表明,在水与碳的摩尔比为5、O_2与碳的摩尔比为0.35、800℃、汽油重时空速0.9 h^(-1)的优化条件下,零售汽油转化率可达100%,产物中 H_2的摩尔分数为69.0%,CH_4的摩尔分数为1.0%,且催化剂的稳定性很好。氢-程序升温还原表征结果显示,被还原的 Pt/CeO_2/Al_2O_3催化剂中 CeO_2表面晶格氧在 O_2中比在水蒸气中容易恢复,因此,自热重整反应中积碳的消除和有机硫的转化能快速进行,从而使催化剂具有良好的稳定性和抗硫中毒性。Effects of reaction parameters, namely n(H2O) : n(C) (C in gasoline) , n(O2) : n(C) , reaction temperature and WHSV of gasoline on performance of Pt/CeO2/Al2O3 catalyst in autothermal reforming (ATR) of retail gasoline with 500 μg/g sulfur were investigated. Catalyst stability in ATR of gasoline was tested in presence of sulfur under optimal reaction conditions. Gasoline conversion of 100% was obtained with H2 mole fraction of 69.0% and CH4 mole fraction of 1.0% in the gas product underthe conditions: 800 ℃, WHSV 0.9 h^-1,n(H2O) : n(C) 5 and n(O2) : n(C) 0.35. The stability of the Pt/CeO2/Al2O3 catalyst in ATR process showed dramatic improvement comparing with steam reforming. The H2-TPR results indicated that Ce^3+ in reduced Pt/CeOJAl2O3 catalyst can retrieve to highly active state of CeO2 by reacting with O2 rather than H2O. In other words, the catalyst can get abundant highly active lattice oxygen from O2 to meet the requirement of coke removal and organo-sulfur conversion thereby leads to good stability and high sulfur resistance.
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