铜基MOF高效催化苯一步氧化制备对苯醌  

One-step oxidation of benzene to p-benzoquinone by highly efficient copper-based MOF

作　　者：侯伟 曾爱武[1,2] HOU Wei;ZENG Aiwu(School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China;State Key Laboratory of Chemical Engineering,Tianjin 300350,China)

机构地区：[1]天津大学化工学院,天津300072 [2]化学工程联合国家重点实验室,天津300350

出　　处：《化学工业与工程》2022年第3期18-25,共8页Chemical Industry and Engineering

摘　　要：采用溶剂热法制备了铜基金属有机骨架材料HKUST-1,并利用XRD、SEM、FTIR、XPS、TG和BET等方法对催化剂进行分析。选取苯氧化生成对苯醌反应作为模型反应,考察了反应温度、反应时间、催化剂用量和氧化剂用量对氧化反应的影响,并筛选了合适的溶剂。实验结果表明,在最适宜反应条件下,对苯醌的选择性和收率分别为64.61%和11.96%;此时催化剂用量为0.15 g,反应温度为60℃,反应时间为80 min,n(苯)∶n(过氧化氢)为1∶4,溶剂为乙腈。此外,催化剂表现出良好的稳定性,反应5次后,对苯醌的收率仍保持在10.87%以上。In this work, the copper-based metal organic framework material HKUST-1 was successfully synthesized by solvothermal method, vigilantly investigated using various techniques including XRD, SEM, FTIR, XPS, TG and BET. The prepared HKUST-1 was applied as a heterogeneous catalyst in oxidation of benzene to p-benzoquinone, and the influence of various reaction conditions such as role of solvents, reaction time and temperature, benzene to hydrogen peroxide molar ratio were specifically investigated. The acquired date manifested that HKUST-1 had shown superiority catalytic performance. Experimental results show that under optimized conditions, 11.96% yield of p-benzoquinone is obtained with the selectivity as high as 64.61%. In addition, the catalyst recovery and reuse test show that HKUST-1 is able to endure the harsh conditions of benzene oxidation for four runs. After the catalyst was recycled 4 times, the yield of p-benzoquinone remained above 10.87%.

关 键 词：苯氧化 对苯醌 HKUST-1 催化 

分 类 号：TQ244.6[化学工程—有机化工]