Cu-xZrO2/SiO2改性催化剂对醋酸甲酯制乙醇性能的影响  

Effect of Cu-xZrO/SiO modified catalyst on the performance of methyl acetate to ethanol

作　　者：徐晨阳 常苏杰 吴涛 刘永梅[1] 申曙光[1] XU Chen-yang;CHANG Su-jie;WU Tao;LIU Yong-mei;SHEN Shu-guang(College of Chemistry and Chemical Engineering,Taiyuan University of Technology,Taiyuan 030024,China)

机构地区：[1]太原理工大学化学化工学院,山西太原030024

出　　处：《天然气化工—C1化学与化工》2020年第5期47-52,共6页Natural Gas Chemical Industry

摘　　要：采用蒸氨法制备一系列ZrO2改性Cu/SiO2催化剂,考察了掺杂不同含量助剂ZrO2对催化剂结构的影响,以及在甲醇裂解制氢中Cu-xZrO2/SiO2催化剂作用下醋酸甲酯制乙醇的反应性能。结果表明,通过引入助剂ZrO2,降低了活性组分的晶粒尺寸,增加了催化剂的比表面积和孔容,提高了活性组分的分散度,特别是有利于层状硅酸铜的形成。在SiO2负载的铜基催化剂上掺杂质量分数为1%的ZrO2时,所制备催化剂(Cu-1ZrO2/SiO2)具有最佳的催化活性,在T=280℃、p=4 MPa、 n(MT)/n(MAC)=4、LHSV=1.8 h-1、 GHSV=120 h-1的反应条件下,甲醇和乙酸甲酯的转化率分别为60.19%和76.79%,催化剂对乙醇的选择性为69.63%,乙醇得率为53.47%。该催化剂既能裂解甲醇产生活性氢,又能促进醋酸甲酯中乙酰基加氢制乙醇,同时降低氢酯比,实现了"一剂两用"。A series of ZrO2 modified Cu/SiO2 catalysts were prepared by the ammonia evaporation method. The effects of different contents of doped additive ZrO2 on the structure of the catalyst and the catalytic performance of Cu-xZrO2/SiO2 catalysts on the methyl acetate to ethanol during hydrogen production from methanol cracking were investigated. The results showed that the introduction of the additive ZrO2 reduced the grain size of the active component, increased the specific surface area and pore volume of the catalyst, and improved the dispersion of the active component. It was particularly beneficial to the formation of layered copper silicate. The catalyst(Cu-1ZrO2/SiO2) has the best catalytic activity as the mass fraction of doped ZrO2 on the SiO2 supported copperbased catalyst was 1%. Under the conditions of T=280 ℃, p=4 MPa, n(MT)/n(MAC)=4, LHSV=1.8 h-1 and GHSV=120 h-1, the conversion of methanol and methyl acetate were 60.19% and 76.79%, respectively. The selectivity of ethanol was 69.63%, and the yield of ethanol was 53.47%. The catalyst can not only crack methanol to produce active hydrogen, but also promote the hydrogenation of acetyl groups in methyl acetate to ethanol and reduces the hydrogen ester ratio to achieve "One dose for two uses".

关 键 词：CU/SIO2催化剂 ZrO2助剂 甲醇裂解 醋酸甲酯加氢 乙醇合成 

分 类 号：O643.3[理学—物理化学]