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以交联聚苯乙烯(CPS)微球为初始物质,通过大分子反应,制备了键合有苯甲醛(BA)的聚合物微球BA-CPS,又以3-氨基吡啶(AP)为试剂,使微球BA-CPS与之发生席夫碱反应,制得了键合有N,N-双齿席夫碱配基的微球BAAP-CPS;然后使微球BAAP-CPS与硫酸氧钒发生配位螯合反应,成功制备了固载有N,N-双齿席夫碱型氧钒(Ⅳ)配合物的微球CPS-[VO(BAAP)2].用红外光谱(FTIR)和固体紫外吸收光谱等手段对微球CPS-[VO(BAAP)2]的化学结构进行了表征.将微球CPS-[VO(BAAP)2]用于乙苯的分子氧催化氧化过程,考察了其催化活性及主要因素对乙苯催化氧化反应的影响,探索研究了催化反应机理.实验结果表明,在分子氧氧化乙苯的反应中,微球CPS-[VO(BAAP)2]具有很高的催化活性和优良的催化选择性,可将乙苯高效地(45%的转化率)转化为单一产物苯乙酮.氧化反应可能遵循自由基反应历程,乙苯侧烷基氢过氧化物可能是关键的中间物.适宜的反应温度为110℃,且体系中催化剂有一适宜用量.
The cross-linked polystyrene (CPS) microspheres were used as the starting materials to prepare the BA-CPS polymer microspheres bonded with the benzaldehyde (BA) via macromolecule reaction. The 3-aminopyridine (AP) , The microsphere BA-CPS was reacted with Schiff base to produce BAAP-CPS microspheres with N, N-bidentate Schiff base ligands. Then BAAP-CPS and vanadyl sulfate The microspheres CPS- [VO (BAAP) 2] immobilized with N, N-bidentate Schiff base vanadyl (Ⅳ) complex were successfully prepared by coordination chelation reaction.FTIR spectroscopy The chemical structure of microspheres CPS- [VO (BAAP) 2] was characterized by UV-Vis absorption spectroscopy etc. The microspheres CPS- [VO (BAAP) 2] were used for the molecular oxygen catalytic oxidation of ethylbenzene Catalytic activity and the main factors on the catalytic oxidation of ethylbenzene were investigated.The catalytic reaction mechanism was explored.The experimental results showed that the microspheres CPS- [VO (BAAP) 2] had high Catalytic activity and excellent catalytic selectivity can convert ethylbenzene efficiently (45% conversion) to acetophenone, a single product.The oxidation reaction may follow the course of the free radical reaction and the ethylbenzene side alkyl hydroperoxide may be The essential Intermediate A suitable reaction temperature is 110 ℃, and the system has a suitable amount of the catalyst.