| Since metal porphyrins were found to be a kind of biomimetic catalyst with high catalytic efficiency, the synthesis of those expensive metal porphyrins has been in progress. Metal porphyrins play a vital important role. in catalytic oxidation of hydrocarbon. Acetophenone and phenylethanol are important intermediates that can be produced by ethylbenzene oxidation in chemical industry. However, it’s difficult to reuse the metal porphyrins in catalytic reaction, because the metal porphyrins will be damaged in homogeneous catalysis system. Therefore, seeking for a green and efficient support to immobilize metal porphyrins becomes the research focus. In this study, a number of nano-porous chitosan boluses （np-CTS） were prepared and used for immobilizing metal tetrakis （p-sulphophenyl） porphyrins （Me TPPSO3H）, forming some nano-porous biomimetic catalytic materials, Me TPPSO3H /np-CTS, which were used to explore catalytic performance and mechanism for oxidation of ethylbenzene. This study includes the following content:1. The research progress about the metal porphyrins, theirs carrier and catalyticoxidation of ethylbenzene is summarized by consulting up related literature.2. Referring to related literature, Metal （Co, Mn and Fe） tetrakis （p-sulphophenyl） porphyrins （Me TPPSO3H） and nano-porous catalyts materials （MeTPPSO3H3+N/np-CTS） were prepared.3. Analyzing and discussing the structure, morphology and stability of the catalyts materials by a variety of characterization methods, such as Ultraviolet-visible spectroscopy （UV-vis）, Fourier transform infrared spectroscopy （FT-IR）, scanning electron microscope （SEM）, X-ray Diffraction pattern （XRD）, Specific area Test （BET） and Thermo-gravimetric analysis （TG）, the structural information of the catalyts materials were obtained.4. Optimzing catalytic reaction conditions （temperature, pressure, amount of catalyst and reaction time） via single-factor experiments to the Me TPPSO3-H3+N/np-CTS and Comparing their catalystic proformance with those of the nano-porous correspongding catalyts materials and the original metal porphyrins, the conclusion is obtained as follows. The size order of catalytic performance is:Me TPPSO3H3+N/np-CTS>Me TPPSO3H>Me TPPSO3-H3+N/nonp-CTS.5. The results show that:nano-porous catalytic materials behave better proformance than the original metal porphyrins and non-porous catalytic materials. Under the optimum catalytic reaction conditions, three kind of metal （Co, Mn, Fe） porphyrin immobilized catalysts can be reused five times. On average, the corresponding conversion rates are 62.88%,61.57% and 52.72%; the yields of alcohol and ketone are 42.91%,39.15% and 33.67%; the selectivities of alcohol and ketone are 68.23%,63.55% and 64.31%, respectively.6. It is initially concludes that the oxidation of ethylbenzene over the catalyst materials is a radical reaction mechanism via analyzing the related experimetal data and referring related literature. |
