环己基苯仿生催化氧化的生物-化学耦合机理与动力学研究

The biomimetic catalytic oxidation of cyclohexylbenzene to phenol and cyclohexanone is a high-effective and green chemical process. In the process, metalloporphyrin is used as the biocatalyst to initiate the reaction, and then the chain will be transfer by the chemical catalyzation of free radical cycle.The biomimitic catalytic oxidation process is coupled with the two types of catalytic effects. By using modern physical and analytical techniques, the detailed bio-chemical coupling mechanism happened in the biomimetic catalytic oxidaiton process will be studies. Firstly, for the biocatalyzed process, the effect of metalloporphyrins structure on the oxidation activity and products selectivities will be investigated. Secondly, for the chemical catalyzed process, the effect of radical cycles on the oxidation activity and products selectivities will be investigated. Thirdly, the structure of the activated intermediates and the reaction process will be in site characterized by using the modern analytical instruments and technologies. Based on the above results, the detailed mechanism for the biomimetic catalytic oxidaton of cyclohexylbenzene to phenol and cyclohexanone will be proposed, and the kinetic expression will be derived. The model parameters in the kinetic models will be determined by the experimental data regression.

针对环己基苯仿生催化氧化联产苯酚和环己酮这个高效和绿色化工过程，运用现代物理和分析技术手段，研究仿生催化氧化过程中的生物催化氧化引发与化学催化自由基循环过程的仿生催化氧化的详细机理。探索用于生物催化的金属卟啉的结构对催化氧化环己基苯的活性与产物选择性的关系问题；探索化学催化过程中自由基循环对金属卟啉仿生催化氧化环己基苯的活性与产物选择性关系；利用现代分析仪器和技术，实现活性中间体结构和反应过程的原位检测，建立工业化仿生催化氧化机理模型；认识金属卟啉催化氧化反应的动力学特征，确立反应工程动力学等环己基苯仿生催化氧化中的基础化学工程问题，为建立高效环己基苯仿生催化氧化工艺和技术提供理论指导。

针对环己基苯仿生催化氧化联产苯酚和环己酮这个高效和绿色化工过程，运用现代物理和分析技术手段，研究了仿生催化氧化过程中的生物催化氧化引发与化学催化自由基循环过程的仿生催化氧化的详细机理，探索了用于生物催化的金属卟啉的结构对催化氧化环己基苯的活性与产物选择性的关系问题，探索了化学催化过程中自由基循环对金属卟啉仿生催化氧化环己基苯的活性与产物选择性关系。利用现代分析仪器和技术，实现了活性中间体结构和反应过程的原位检测，建立了工业化仿生催化氧化机理模型，认识了金属卟啉催化氧化环己基苯的反应动力学特征，确立了反应工程动力学等环己基苯仿生催化氧化中的基础化学工程问题，为建立高效环己基苯仿生催化氧化工艺和技术提供了理论指导。