| ZrO2-Al2O3复合氧化物催化反应精馏合成碳酸二甲酯 |
| |
| 引用本文： | 陶宁,徐亚津,冯宇辰,吕建华,刘继东. ZrO2-Al2O3复合氧化物催化反应精馏合成碳酸二甲酯[J]. 化工进展, 2021, 40(5): 2603-2612. DOI: 10.16085/j.issn.1000-6613.2020-0573 |
| |
| 作者姓名： | 陶宁 徐亚津 冯宇辰 吕建华 刘继东 |
| |
| 作者单位： | 河北工业大学化工学院,天津300130 |
| |
| 摘 要： | 采用共沉淀法制备了一系列不同Al2O3含量的ZrO2-Al2O3复合氧化物，并在催化精馏实验装置中考察了该催化剂在碳酸丙烯酯（PC）与甲醇酯交换制备碳酸二甲酯（DMC）过程中的催化性能。通过X射线衍射（XRD）、红外光谱（FTIR）、X射线光电子能谱（XPS）、CO2程序升温脱附（CO2-TPD）和NH3程序升温脱附（NH3-TPD）等手段对所制备的催化剂进行了表征。结果表明，催化剂表面存在的酸碱性位点是制约PC与甲醇酯交换性能的重要因素。复合氧化物中Al2O3含量可以有效调控催化剂的结构特征和表面的酸碱性质，不同于ZrO2或Al2O3单金属催化剂，复合氧化物ZrO2-Al2O3在合成过程中形成了稳定的固溶体结构，导致催化剂表面弱酸量增加，并产生了强碱位点。数据分析表明，催化剂表面的强碱和弱酸含量高时，其催化活性高，说明该反应具有酸碱协同催化作用。当Zr/Al比为1时，弱酸和强碱量均达到最大值，PC的转化率和DMC选择性可达到98.14%和99.96%。催化剂在经过12次循环使用后依旧保持较高的活性，具有良好的结构稳定性。
|
| 关 键 词： | ZrO2-Al2O3复合氧化物 酯交换 碳酸二甲酯 酸碱协同 |
| 收稿时间： | 2020-04-13 |
ZrO2-Al2O3 composite oxide for synthesis of dimethyl carbonate in catalytic reactive distillation |
| |
| TAO Ning,XU Yajin,FENG Yuchen,LYU Jianhua,LIU Jidong. ZrO2-Al2O3 composite oxide for synthesis of dimethyl carbonate in catalytic reactive distillation[J]. Chemical Industry and Engineering Progress, 2021, 40(5): 2603-2612. DOI: 10.16085/j.issn.1000-6613.2020-0573 |
| |
| Authors: | TAO Ning XU Yajin FENG Yuchen LYU Jianhua LIU Jidong |
| |
| Affiliation: | College of Chemical Engineering, Hebei University of Technology, Tianjin 300130, China |
| |
| Abstract: | A series of ZrO2-Al2O3 composite oxides with different Al2O3 contents were prepared by coprecipitation method. Then, the catalytic performance of these catalysts in the process of transesterification of propylene carbonate (PC) and methanol to synthesize dimethyl carbonate (DMC) was investigated in the catalytic distillation experiment. The catalysts were characterized by XRD, FTIR, XPS, CO2-TPD and NH3-TPD. The results show that the presence of acid-base sites on the catalyst surface is the key factor for the restriction of the transesterification of PC and methanol. Different from ZrO2 or Al2O3 single metal catalysts, the synthesized ZrO2-Al2O3 catalysts form a stable solid solution structure. The amount of weak acid increased and strong base sites were produced on the catalyst surface. Data analysis shows that when the content of strong base and weak acid on the surface of the catalyst is high, its catalytic activity is high, indicating that the reaction has a synergistic catalytic effect of acid and base. When the Zr/Al ratio is 1, the contents of weak acid and strong base reach the maximum level, and the conversion and DMC selectivity of PC can reach 98.14% and 99.96%. After 12 cycles of recycling, the catalyst still has high activity and presents remarkable good structural stability. |
| |
| Keywords: | ZrO2-Al2O3 composite oxides transesterification dimethyl carbonate acid-base synergistic |
| 本文献已被 万方数据 等数据库收录！ |
| 点击此处可从《化工进展》浏览原始摘要信息 |
|
点击此处可从《化工进展》下载免费的PDF全文 |
|
