甲醇水蒸气重整制氢CuO/CeO2-ZrO2/SiC整体催化剂的研究  

Research on CuO/CeO2-ZrO2/SiC monolithic catalysts for hydrogen production from steam reforming of methanol

作　　者：焦桐 许雪莲 张磊[1] 翁幼云 翁玉冰 高志贤 JIAO Tong;XU Xue-lian;ZHANG Lei;WENG You-yun;WENG Yu-bing;GAO Zhi-xian(School of Petrochemical Engineering,Liaoning Shihua University,Fushun 113001,China;Guizhou Muyee Fine Ceramics Company Limited,Guiyang 550000,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]贵州木易精细陶瓷有限公司,贵州贵阳550000

出　　处：《燃料化学学报》2020年第9期1122-1130,I0007,共10页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21673270)资助。

摘　　要：采用浸渍法和溶胶凝胶法制备了CuO/CeO2-ZrO2/SiC整体催化剂,并将其用于甲醇水蒸气重整制氢反应中。结果表明,与CuO/CeO2-ZrO2颗粒催化剂相比,CuO/CeO2-ZrO2/SiC整体催化剂催化活性较好,产氢速率较快且重整气中CO体积分数较低。进一步探究了涂层涂覆量和CuO负载量对催化性能的影响,结果表明,当CeO2-ZrO2复合氧化物涂层涂覆量在15%±1%,CuO负载量为5%±1%时,催化性能较好;当反应温度为340℃,水醇物质的量比为1.2,甲醇水蒸气气体空速为4840h^-1时,甲醇转化率为86.0%,产氢速率为1490.0L/(m^3·s),重整气中CO体积分数为1.55%。最后通过单因素实验法探究了甲醇水蒸气气体空速、水醇物质的量比和反应温度对反应的影响。结果表明,随着气体空速变大,甲醇转化率下降,产氢速率上升,重整气中CO体积分数下降。随着水醇物质的量比增加,甲醇转化率先上升后下降,产氢速率先上升后下降,重整气中CO体积分数下降。随着反应温度的升高,甲醇转化率、产氢速率和重整气中CO体积分数均上升。CuO/CeO 2-ZrO 2/SiC monolithic catalysts were prepared by the sol-gel and incipient-wetness impregnation methods,and then used in methanol steam reforming reaction for H 2 production.The results indicated that CuO/CeO 2-ZrO 2/SiC monolithic catalysts showed better activity,higher hydrogen production rate and less CO volume fraction than the CuO/CeO 2-ZrO 2 bead catalysts.Then the effects of CuO content and coating amount on methanol steam reforming were explored.When the CeO 2-ZrO 2 mass content was 15%±1%and CuO was 5%±1%,the obtained catalyst showed the best catalytic activity.At a reaction temperature of 340℃,water and methanol molar ratio of 1.2,methanol and water gas hourly space velocity of 4840 h^-1,methanol conversion reached 86.0%,hydrogen production rate was 1490.0 L/(m^3·s),and CO content in reformed gas was 1.55%.The effects of gas hourly space velocity,water and methanol molar ratio and temperature on methanol steam reforming reaction activity were studied by the single factor experiments.The results showed that,as the gas hourly space velocity increased,methanol conversion decreased,hydrogen production rate increased,and the volume fraction of CO in the reformed gas decreased.As the molar ratio of water to methanol increased,both the methanol conversion and the hydrogen production rate increased first and then declined,and the volume fraction of CO in the reformed gas decreased.With the increase of reaction temperature,methanol conversion rate,hydrogen production rate and the content of CO in the reformed gas increased.

关 键 词：甲醇水蒸气重整 氢气 一氧化碳 整体催化剂 

分 类 号：O643[理学—物理化学]