Cu-Fe-MgO/AlPO_4-5对甲醇水蒸气重整制氢的催化性能研究  

Study on catalytic properties of Cu-Fe-MgO/AlPO_4-5 for hydrogen production from steam reforming of methanol

作　　者：巢磊[1] 武丹丹[1] 李工[1] 

机构地区：[1]常州大学石油化工学院,江苏常州213164

出　　处：《燃料化学学报》2017年第9期1105-1113,共9页Journal of Fuel Chemistry and Technology

摘　　要：以AlPO_4-5分子筛为载体,采用浸渍法制备Cu-Fe-MgO/AlPO_4-5催化剂,用于催化甲醇和水蒸气重整反应制氢气。采用XRD、N2吸附-脱附、H2-TPR、CO2-TPD和NH3-TPD等对催化剂进行表征。结果表明,加入Fe可以明显提高甲醇的转化率,但副产物二甲醚的选择性也增加,添加MgO对降低二甲醚具有明显的作用,但不能提高甲醇的转化率。AlPO_4-5负载Cu、Fe和MgO的质量分数分别为15%、6%和1%时具有较高的催化活性,在反应温度300℃、水醇物质的量比为1.1∶1和质量空速2.51 h^(-1)的条件下,对甲醇的转化率为93.08%,二氧化碳和氢气的选择性分别为95.80%和96.93%,对副产物一氧化碳和二甲醚的选择性分别为1.70%和2.51%。表征结果表明,Cu-Fe-MgO/AlPO_4-5同时含有弱酸弱碱和强酸强碱中心,适量的MgO增加了强碱中心的量,降低弱酸中心的强度,但对强酸中心影响不大。Cu-Fe-MgO/AlPO4-5 catalysts were prepared by impregnation method using AlPO4-5 molecular sieve as support to produce hydrogen through steam reforming of methanol.The catalysts were characterized by XRD,N2 adsorption-desorption,H2-TPR,CO2-TPD and NH3-TPD.The reaction results indicated that the addition of Fe could significantly increase the conversion of methanol,but the selectivity of dimethyl ether was also increased.The addition of MgO had obvious effects on the reduction of dimethyl ether formation,but the conversion of methanol could not be improved.The catalyst with Cu,Fe and MgO loadings of 15%,6% and 1%,respectively showed a higher catalytic activity.Under the reaction conditions of 300 ℃,1.1∶1 of molar ratio of water to alcohol and 2.51 h^-1 of mass space velocity,the conversion of methanol was 93.08%,the selectivity of carbon dioxide and hydrogen were 95.80% and 96.93% respectively and the selectivity of by-products of carbon monoxide and dimethyl ether were 1.70% and 2.51% respectively.According to the characterization results,Cu-Fe-MgO/AlPO4-5 contains weak acid and base sites,strong acid and base sites.It can be concluded that appropriate amount of MgO increases the amount of strong basic sites,reduces the strength of weak acidic sites,but had little effects on strong acidic sites.

关 键 词：AlPO4-5分子筛 Cu-Fe-MgO/AlPO4-5 催化反应 甲醇水蒸气重整 氢气 

分 类 号：O643[理学—物理化学]