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Efficient oxidation of cycloalkanes with simultaneously increased conversion and selectivity using O2 catalyzed by metalloporphyrins and boosted by Zn(AcO)2: A practical strategy to inhibit the formation of aliphatic diacids
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2020-11-02 , DOI: 10.1016/j.apcata.2020.117904
Hai-Min Shen , Xiong Wang , Lei Ning , A-Bing Guo , Jin-Hui Deng , Yuan-Bin She

The direct sources of aliphatic acids in cycloalkanes oxidation were investigated, and a strategy to suppress the formation of aliphatic acids was adopted through enhancing the catalytic transformation of oxidation intermediates cycloalkyl hydroperoxides to cycloalkanols by Zn(II) and delaying the emergence of cycloalkanones. Benefitted from the delayed formation of cycloalkanones and suppressed non-selective thermal decomposition of cycloalkyl hydroperoxides, the conversion of cycloalkanes and selectivity towards cycloalkanols and cycloalkanones were increased simultaneously with satisfying tolerance to both of metalloporphyrins and substrates. For cyclohexane, the selectivity towards KA-oil was increased from 80.1% to 96.9% meanwhile the conversion was increased from 3.83 % to 6.53 %, a very competitive conversion level with higher selectivity compared with current industrial process. This protocol is not only a valuable strategy to overcome the problems of low conversion and low selectivity lying in front of current cyclohexane oxidation in industry, but also an important reference to other alkanes oxidation.



中文翻译:

使用金属卟啉和Zn(AcO)2促进的O 2高效氧化环烷烃,同时提高转化率和选择性:抑制脂肪族二酸形成的实用策略

研究了环烷烃氧化中脂肪酸的直接来源,并采取了抑制脂族酸形成的策略,该方法通过增强氧化中间体环烷基氢过氧化物通过Zn(II)催化转化为环烷醇和延迟环烷酮的出现而采取了抑制策略。得益于环烷酮的延迟形成和环烷基氢过氧化物的非选择性热分解,环烷的转化率和对环烷醇和环烷酮的选择性同时提高,同时满足了对金属卟啉和底物的耐受性。对于环己烷,对KA油的选择性从80.1%增加到96.9%,同时转化率从3.83%增加到6.53%,与目前的工业流程相比,具有很高的选择性和更高的竞争力。该方案不仅是克服目前环己烷氧化工业面临的转化率低和选择性低的问题的有价值的策略,而且是其他烷烃氧化的重要参考。

更新日期:2020-11-13
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