丁二酸插层S_2O_8^(2-)/Mg-Al水滑石的制备及催化环己酮自缩合反应  

Preparation of Succinic Acid Pillared S_2O_8^(2-)/Mg-Al Hydrotalcites and their Application in Cyclohexanone Self-Condensation

作　　者：任晓乾[1] 孙守飞[1] 梁金花[2] 陈刘龙 王俊格[1] 姜岷[2] 

机构地区：[1]南京工业大学化学化工学院,江苏南京210009 [2]南京工业大学生物与制药工程学院,江苏南京211816

出　　处：《高校化学工程学报》2015年第4期866-872,共7页Journal of Chemical Engineering of Chinese Universities

基　　金：国家重点基础研究规划(973计划)资助项目(2009CB724701);国家高技术研究发展计划(863计划)资助项目(2014AA021205)

摘　　要：开发出了一系列具有较高转化率和选择性的适用于环己酮缩合反应的固体催化剂,采用浸渍法、焙烧复原法制备S-2O28/Su-Mg Al水滑石,利用XRD、FT-IR、BET、SEM对所制催化剂进行了表征。有机酸根插层S2O2-8改性后的镁铝水滑石仍保持原有的层状骨架结构;S2O2-8改性后,水滑石酸性增强,使水滑石成为具有酸碱双功能的催化剂。以环己酮自缩合反应为探针反应,考察了催化剂的催化性能。当(NH4)2S2O8浸渍液浓度为1.0 mol?L-1,催化剂用量为环己酮质量的5.0%(wt),甲苯为带水剂,140℃下反应6 h时,环己酮转化率可达85.7%,二聚物选择性可达89.6%,活性优于Mg-Al水滑石(5.6%)和丁二酸根插层水滑石(53.4%),该催化剂对环己酮自缩合反应显示出较高的催化活性,体现出了明显的酸碱协同催化作用。A series of solid catalysts with high conversion performance and excellent selectivity for cyclohexanone self-condensation were developed. S2O8^2-/Su-MgA1 hydrotalcites were prepared by impregnation and reconstruction methods and their structures were characterized by XRD, FT-IR, BET and SEM. The results show that no significant structural change of LDH was observed after modification. The catalyst acidity was strengthened and acid-base bi-functional LDH catalysts can be obtained. The catalytic performance of these catalysts was tested on cyclohexanone self-condensation. The results show that cyclohexanone conversion rate of 85.7% and selectivity of 89.6% can be achieved under experimental conditions of 1.0 mol·L^-1 （NH4）2S2O8 solution, 140℃, 6 h and catalyst dosage of 5.0% （based on the weight of cyclohexanone）. The catalytic activity of the succinic acid pillared S2O8^2-/Mg-Al hydrotalcites was better than that of LDH（5.6%） and succinic acid pillared hydrotalcites （53.4%）. The novel succinic acid pillared S2O8^2-/Mg-Al hydrotalcite catalysts show good catalytic performance in cyclohexanone self-condensation and exhibit acid-base coordination processes.

关 键 词：类水滑石 过硫酸铵 酸碱双功能 环己酮 自缩合 

分 类 号：O643[理学—物理化学]