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以Cu、Zn、Ni为活性金属中心,活性碳(AC)为载体,通过正交实验设计,筛选获得了具有较好羰基化性能的ZnCuNi/AC,其中3种活性组分的最佳含量依次为6%、9%和3%(mas)。活性评价表明:在该催化剂体系中,ZnCuNi/AC催化丙醇羰基化反应合成羧酸和酯的总收率达3087%(mass),催化活性明显高于其它配比的催化剂,而且催化活性的高低与催化剂中3种活性金属的相对含量密切相关,Cu(I)的存在有利于羧酸的形成,Zn的加入可抑制Ni对反应物的裂解力;其次还考察了工艺条件对ZnCuNi/AC催化剂性能的影响,结果发现低温有利于丙醇反应生成羧酸,较高温度有利于酯类的生成,随着空速的提高羧酸/酯之比略有增加,但催化剂活性下降。
With Cu, Zn, Ni as the active metal center and activated carbon (AC) as carrier, ZnCuNi / AC with good carbonylation performance was screened through orthogonal experimental design, of which three active components The best content is 6%, 9% and 3% (mas). The activity evaluation showed that in the catalyst system, Zn-Cu-Ni / AC catalyzed the overall yield of carboxylic acid and ester synthesized by carbonylation of propanol to 3087% (mass), and the catalytic activity was significantly higher than that of the other compounds The catalytic activity is closely related to the relative content of the three active metals in the catalyst. The presence of Cu (I) favors the formation of carboxylic acids. The addition of Zn inhibits the cracking of Ni on the reactants. Secondly, The effect of process conditions on the performance of ZnCuNi / AC catalysts was studied. It was found that low temperature was conducive to the reaction of propanol with carboxylic acid. Higher temperature was favorable for the formation of esters. With the increase of space velocity, the ratio of carboxylic acid to ester There is an increase, but the activity of the catalyst is decreased.