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化学工业与工程 2022, Vol. 39 Issue (3) :18-25    DOI: 10.13353/j.issn.1004.9533.20210321
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铜基MOF高效催化苯一步氧化制备对苯醌
侯伟1, 曾爱武1,2
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
One-step oxidation of benzene to p-benzoquinone by highly efficient copper-based MOF
HOU Wei1, ZENG Aiwu1,2
1. School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2. State Key Laboratory of Chemical Engineering, Tianjin 300350, China

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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。
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侯伟
曾爱武
关键词苯氧化   对苯醌   HKUST-1   催化     
Abstract: 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%.
Keywordsbenzene oxidation   p-benzoquinone   HKUST-1   catalysis     
Received 2021-03-24;
Corresponding Authors: 曾爱武,副研究员,E-mail:awzeng@tju.edu.cn。     Email: awzeng@tju.edu.cn
About author: 侯伟(1995-),男,硕士研究生,现从事苯氧化反应方面的研究。
引用本文:   
侯伟, 曾爱武.铜基MOF高效催化苯一步氧化制备对苯醌[J].  化学工业与工程, 2022,39(3): 18-25
HOU Wei, ZENG Aiwu.One-step oxidation of benzene to p-benzoquinone by highly efficient copper-based MOF[J].  Chemcial Industry and Engineering, 2022,39(3): 18-25
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