异辛烷蒸汽重整制氢的研究 Ⅱ.抗硫中毒Pt/CeO_2/Al_2O_3催化剂的程序升温还原表征  被引量:7

Steam Reforming of iso-Octane for Hydrogen Production Ⅱ.H_2-TPR Characterization of Sulfur Tolerant Pt/CeO_2/Al_2O_3 Catalyst

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作  者:薛青松[1] 高立达[1] 陈金春[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5期439-444,共6页Petrochemical Technology

基  金:国家自然科学基金项目(20590366;20573036);"863"计划项目(2007AA05Z101);上海市科委重大基础科研计划项目(05DJ14002);新世纪优秀人才支持计划项目(06-NCET-0423);上海市重点学科建设资助项目(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:利用程序升温还原方法研究了Pt/CeO2/Al2O3催化剂中Pt与CeO2/Al2O3载体间的强相互作用,考察了γ-Al2O3、CeO2/Al2O3载体和Pt/CeO2/Al2O3催化剂焙烧温度、Pt和CeO2负载量对催化剂还原行为的影响。表征结果显示,用800℃焙烧的γ-Al2O3负载质量分数15%的CeO2,再在450℃焙烧后制备的CeO2/Al2O3载体的CeO2还原活性最好,以该载体负载质量分数0.8%的Pt,再在600℃焙烧后制备的Pt/CeO2/Al2O3催化剂为最优化催化剂。该催化剂中Pt-CeO2间形成较强的相互作用,Pt分散性好,从而显著促进表面CeO2的还原及Pt-Ce-Al三者间形成较好的协同作用。在异辛烷蒸汽重整反应中,这种协同作用可能对有机硫快速转化生成H2S有促进作用,从而抑制硫物种在催化剂表面的沉积。H2-TPR of Pt/CeO2/Al2O3 catalysts was carried out to reveal strong interaction between Pt and support CeO2/Al2O3. Calcination temperature of γ-Al2O3, CeO2/Al2O3, Pt/CeO2/Al2O3 and Pt ( or CeO2 ) loading were factors influencing reduction behavior of the catalysts. Under the conditions : γ-Al2O3 calcination temperature 800 ℃, which was loaded with 15% (mass fraction)of CeO2, the resulted CeO2/Al2O3 support calcination temperature 450 ℃, the reduction activity of CeO2 was remarkable. Loading of 0.8 % ( mass fraction) Pt on the CeO2/Al2O3 support, followed by successive calcination at 600 ℃, and then the most active catalyst Pt/CeO2/Al2O3 was obtained. Strong interaction between Pt and CeO2 facilitates the dispersion of Pt, which leads to significant promotion of N-catalyzed reduction of CeO2. It is suggested that obvious synergistic effect among Pt-Ce-Al exists in this optimal catalyst. In steam reforming it may accelerate the sulfur conversion into H2S which is easily to escape and therefore deposition of poisonous sulfur species on the catalyst surface can be greatly avoided.

关 键 词:程序升温还原  氧化铈 氧化铝 抗硫中毒催化剂 异辛烷 蒸汽重整 制氢 

分 类 号:TQ426.8[化学工程]

 

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