| 制备方法对ZnO-ZrO2催化剂上乙醇转化制异丁烯反应的影响 |
| Influence of Preparative Method on ZnO-ZrO2 Catalyst for Ethanol Conversion to Isobutene |
| 作者 | 单位 | E-mail | | 刘田 | 复旦大学化学系, 上海市分子催化和功能材料重点实验室, 上海 200433 | | | 薛芳琦 | 复旦大学化学系, 上海市分子催化和功能材料重点实验室, 上海 200433 | | | 乐英红 | 复旦大学化学系, 上海市分子催化和功能材料重点实验室, 上海 200433 | | | 华伟明 | 复旦大学化学系, 上海市分子催化和功能材料重点实验室, 上海 200433 | wmhua@fudan.edu.cn | | 高滋 | 复旦大学化学系, 上海市分子催化和功能材料重点实验室, 上海 200433 | |
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| 摘要: 采用恒pH值共沉淀法和非恒pH值共沉淀法制备了ZnO-ZrO2混合氧化物催化剂，考察了制备方法对乙醇转化制异丁烯反应的影响，并用低温N2吸附、X射线衍射、扫描电子显微镜、透射电子显微镜、X射线光电子能谱、拉曼光谱、紫外-可见漫反射光谱、NH3程序升温脱附和CO2程序升温脱附对催化剂进行了表征。研究结果表明，相比于非恒pH值共沉淀法制备的ZnO-ZrO2，恒pH值共沉淀法制备的ZnO-ZrO2具有较高的比表面积，更多的酸量和碱量，从而表现出更好的乙醇转化制异丁烯催化性能。在450℃和乙醇质量空速0.2 h-1的反应条件下，两种催化剂的乙醇转化率均为100%，恒pH值共沉淀法制备的催化剂的异丁烯得率为54.9%，明显高于非恒pH值共沉淀法制备的催化剂(45.7%)，并且稳定性也是前者明显高于后者。 |
| 关键词: 混合氧化物 制备方法 乙醇 异丁烯 酸碱性 |
| 基金项目: 国家自然科学基金（No.21273043）和上海市科委资助项目（No.13DZ2275200）资助。 |
| Abstract: ZnO-ZrO2 mixed oxide catalysts were prepared using either a constant or variable pH value co-precipitation method. The obtained catalyst samples were characterized using N2 adsorption, X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, ultraviolet-visible diffuse reflectance, NH3 temperature-programmed desorption and CO2 temperature-programmed desorption. Compared to the ZnO-ZrO2 mixed oxide prepared using the variable pH value method, the corresponding mixed oxide prepared using the constant pH value method had a higher surface area and a higher number of acid sites and basic sites, thus exhibiting a superior catalytic performance. When the reaction temperature was 450℃ and the weight hourly space velocity of ethanol was 0.2 h-1, the conversion of ethanol for both catalysts was 100%. The ZnO-ZrO2 catalyst prepared using the constant pH value method gave 54.9% yield of isobutene, which was obviously greater than the yield obtained using the corresponding catalyst prepared using the variable pH value method (45.7%). Moreover, the former catalyst exhibited obviously higher stability than the latter one for the isobutene production from ethanol conversion. |
| Keywords: mixed oxide preparative method ethanol isobutene acidity and basicity |
| 投稿时间：2016-01-31 修订日期：2016-05-11 |
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| 刘田,薛芳琦,乐英红,华伟明,高滋.制备方法对ZnO-ZrO2催化剂上乙醇转化制异丁烯反应的影响[J].无机化学学报,2016,32(8):1391-1397. |
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