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The Selective Oxidation of Cyclohexane via In-situ H2O2 Production Over Supported Pd-based Catalysts
Catalysis Letters ( IF 2.3 ) Pub Date : 2021-01-18 , DOI: 10.1007/s10562-020-03511-6
Caitlin M. Crombie , Richard J. Lewis , Dávid Kovačič , David J. Morgan , Thomas J. A. Slater , Thomas E. Davies , Jennifer. K. Edwards , Martin Skov Skjøth-Rasmussen , Graham J. Hutchings

The oxidation of cyclohexane via the in-situ production of H2O2 from molecular H2 and O2 offers an attractive route to the current industrial means of producing cyclohexanone and cyclohexanol (KA oil), key materials in the production of Nylon. The in-situ route has the potential to overcome the significant economic and environmental concerns associated with the use of commercial H2O2, while also allowing for the use of far lower reaction temperatures than those typical of the purely aerobic route to KA oil. Herein we demonstrate the efficacy of a series of bi-functional Pd-based catalysts, which offer appreciable concentrations of KA oil, under conditions where limited activity is observed using O2 alone. In particular the introduction of V into a supported Pd catalyst is seen to improve KA oil concentration by an order of magnitude, compared to the Pd-only analogue. In particular we ascribe this improvement in catalytic performance to the development of Pd domains of mixed oxidation state upon V incorporation as evidenced through X-ray photoelectron spectroscopy.

中文翻译:

在负载型 Pd 基催化剂上通过原位 H2O2 选择性氧化环己烷

通过从分子 H2 和 O2 原位生产 H2O2 氧化环己烷为目前生产环己酮和环己醇(KA 油)的工业手段提供了一条有吸引力的途径,环己酮和环己醇是尼龙生产的关键材料。原位路线有可能克服与使用商业 H2O2 相关的重大经济和环境问题,同时还允许使用比典型的纯有氧路线用于 KA 油的反应温度低得多的反应温度。在此,我们展示了一系列双功能 Pd 基催化剂的功效,这些催化剂可在仅使用 O2 观察到活性有限的条件下提供可观的 KA 油浓度。特别是将 V 引入负载型 Pd 催化剂被认为可以将 KA 油浓度提高一个数量级,与仅 Pd 的类似物相比。特别地,我们将催化性能的这种改进归因于 V 掺入后混合氧化态 Pd 域的发展,如 X 射线光电子能谱所证明的那样。
更新日期:2021-01-18
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