SO_4^(2-)/ZrO_2-SiO_2 超强酸催化剂研究 (Ⅰ)—制备及对乙酸/丁醇酯化反应的催化活性(英文)

Study on the Superacid Catalyst SO_4^(2-)/ZrO_2-SiO_2(Ⅰ) —Preparation and Activity for Esterification of Acetic Acid with Butanol

采用 0 .3～ 2 .0mol/dm3的硫酸水溶液浸渍预焙烧过的二元氧化物 ,然后在 4 50～ 6 50℃的温度下焙烧 3～ 5h ,制得SiO2 /ZrO2 摩尔比为 1∶9～ 30的SO4 2 - /ZrO2 -SiO2 催化剂 .ZrO2 -SiO2 二元氧化物前体由沉淀 /混合沉淀法制得 .对于乙酸 /丁醇酯化反应 ,所制得的催化剂的活性比传统的SO2 - 4/ZrO2 催化剂高 6～ 10倍 .考察了SiO2 /ZrO2 摩尔比 ,硫酸水溶液浓度 ,预焙烧温度和焙烧温度等制备条件对催化剂活性的影响 .SiO2 /ZrO2 摩尔比为 10～ 15,以 1.0mol/dm3硫酸溶液浸渍 ,且在 550℃温度下焙烧制得的催化剂表现出最好的催化活性 .

A new type of superacid catalysts, SO 2- 4/ZrO 2-SiO 2, in which the molar ratios of SiO 2/ZrO 2 range from 0.11 to 30, has been prepared by impregnating the pre_calcined binary oxides with 0.3 to 2.0 mol/dm 3 H 2SO 4 aqueous solutions, followed by calcining at 450 to 650℃ for 3 to 5 hours. The precursor ZrO 2-SiO 2 binary oxides were prepared by a precipitating/mixing_precipitate method. The prepared catalyst showed an activity six to ten times higher than the traditional SO 2- 4/ZrO 2 catalyst for the esterification of acetic acid with butanol. The effects of some preparation conditions, such as the molar ratio of SiO 2/ZrO 2, the concentration of H 2SO 4 aqueous solution, the pre_calcining temperature and calcination temperature on the catalytic activity were investigated. The catalyst with ratio of SiO 2/ZrO 2 of 10 to 15 and soaked with 1.0 mol/dm 3 sulfuric acid solution and calcined at 550 ℃ showed the best activity.