MIL-100(Fe)催化正戊醛自缩合反应性能  

MIL-100(Fe) Catalyzed Self-Condensation of n-Valeraldehyde

作　　者：王娣 李步卫 安华良[1] 赵新强[1] 王延吉[1] WANG Di;LI Bu-wei;AN Hua-liang;ZHAO Xin-qiang;WANG Yan-ji(Hebei Provincial Key Laboratory of Green Chemical Technology and Efficient Energy Saving,School of Chemieal Engineering and Technology,Hebei University of Technology,Tianjin 300130,China)

机构地区：[1]河北工业大学化工学院绿色化工与高效节能河北省重点实验室,天津300130

出　　处：《精细化工》2019年第1期94-100,共7页Fine Chemicals

基　　金：国家自然科学基金(21506046;21476058);天津市自然科学基金青年项目(16JCQNJC06100)~~

摘　　要：以硝酸铁和1,3,5-苯三甲酸为原料,采用水热法制备了金属有机骨架材料MIL-100(Fe)催化剂,采用XRD、SEM、BET对其结构进行了表征。评价了MIL-100(Fe)催化正戊醛自缩合合成2-丙基-2-庚烯醛的反应性能。根据GC-MS分析结果,推测了该反应体系中的副产物以及可能发生的副反应。通过条件优化实验,得到适宜的反应条件为:催化剂用量为15%(以正戊醛的质量为基准,下同)、反应温度为130℃、反应时间为8 h。在该条件下,正戊醛转化率为73.5%,2-丙基-2-庚烯醛收率和选择性分别为63.2%和86.0%。MIL-100(Fe)催化剂重复使用4次后,催化活性没有明显下降,通过XRD、FTIR分析证明其催化剂结构未发生坍塌。建立了MIL-100(Fe)催化正戊醛自缩合反应网络。Metal-organic framework MIL-100(Fe) catalyst was prepared by hydrothermal method using ferric nitrate and benzene tricarboxylic acid as raw materials.Its structure was characterized by XRD,SEM and BET.Its catalytic performance for n-valeraldehyde self-condensation to 2-propyl-2-heptenal was evaluated.According to the results of GC-MS analysis,the by-products and possible side reactions in the reaction system were speculated.The effect of reaction conditions on 2-propyl-2-heptenal synthesis was investigated and the suitable reaction conditions were determined as follows:a weight percentage of MIL-100(Fe)=15%(benchmarked against the quality of n-valeraldehyde,the following is the same),a reaction temperature of 130 ℃,and a reaction time of 8 h.Under the above conditions,the conversion of n-valeraldehyde was 73.5%,the yield and selectivity of 2-propyl-2-heptenal were 63.2% and 86.0%,respectively.The MIL-100(Fe) catalyst could be reused for four times without a significant loss in its catalytic performance.XRD and FTIR analysis showed that the catalyst structure did not collapse.Lastly,a possible reaction network of MIL-100(Fe) catalyzed n-valeraldehyde self-condensation was established.

关 键 词：正戊醛 羟醛缩合 2-丙基-2-庚烯醛 MIL-100(Fe) 反应网络 催化技术 

分 类 号：TQ203.2[化学工程—有机化工]