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甲醇水蒸气重整制氢反应条件的优化

Optimization of methanol steam reforming for hydrogen production

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【作者】 张磊潘立卫倪长军赵生生王树东胡永康王安杰蒋凯

【Author】 ZHANG Lei1,2,PAN Li-wei1,NI Chang-jun1,ZHAO Sheng-sheng1, WANG Shu-dong1,HU Yong-kang3,WANG An-jie2,JIANG Kai1(1.Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China; 2.State Key Laboratory of Fine Chemicals,Dalian University of Technology,Dalian 116023,China; 3.Fushun Research Institute of Petroleum and Petrochemicals,Fushun 113001,China)

【机构】 中国科学院大连化学物理研究所大连理工大学精细化工国家重点实验室抚顺石油化工研究院

【摘要】 对共沉淀法制备的CuO/ZnO/CeO2-ZrO2催化剂在甲醇水蒸气重整制氢反应体系中的性能进行了考察,并利用统计学实验设计方法对该反应的反应条件进行了优化。选择反应温度、水醇比和甲醇气体空速为独立要因,利用全因子实验设计方法,得到反应温度对两个响应值(甲醇转化率和重整气中CO物质的量分数)的影响最为显著,甲醇气体空速对重整气中CO物质的量分数的影响最小。固定甲醇气体空速为300 h-1,利用中心旋转组合设计实验方法对反应温度和水醇比进行优化,得出当反应温度在249~258℃、水醇比在1.76~2.00时,甲醇能全部转化,重整气中CO物质的量分数小于0.5%。此模型的计算值与实验结果较为接近,表明采用统计学实验设计方法得出的结论对甲醇水蒸气重整制氢反应条件的优化具有指导意义。

【Abstract】 The catalytic performance of CuO/ZnO/CeO2/ZrO2 prepared by co-precipitation for methanol steam reforming was investigated using a statistical set of experiments in order to optimize the reaction conditions for obtaining minimal carbon monoxide in the reformed gas.The reaction temperature,steam to methanol ratio,methanol gas hourly space velocity(GHSV) were evaluated with a full factorial design experiment.The reaction temperature displayed much greater influence on the response(methanol conversion and CO concentration in reformed gas),GHSV has minimal influence on the CO concentration in reformed gas.At a fixed low methanol GHSV(300 h-1),a central composite rotatable design was then used to approximate the optimal conditions by simultaneously considering the methanol conversion and CO concentration.The optimum theoretical conditions were found to lie within a reaction temperature of 249-258 ℃ and a W/M ratio of 1.76-2.00,in close agreement with the experimental results.

【基金】 国家自然科学基金(21076206);国家重点基础研究发展规划(973计划,2010CB732302);国家高技术研究发展计划(863计划,2011AA050706)
  • 【文献出处】 燃料化学学报 ,Journal of Fuel Chemistry and Technology , 编辑部邮箱 ,2013年01期
  • 【分类号】TQ116.2
  • 【被引频次】13
  • 【下载频次】713
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