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Novel high TEMPO loading magneto-polymeric nanohybrids: An efficient and recyclable Pickering interfacial catalyst
Journal of Catalysis ( IF 6.5 ) Pub Date : 2017-08-07 , DOI: 10.1016/j.jcat.2017.07.020
Jun Tang , Qi Zhang , Kecheng Hu , Peng Zhang , Jianli Wang

We report herein the design and preparation of novel magneto-polymeric nanohybrids that can be used as efficient and recyclable Pickering interfacial catalyst (PIC) in selective oxidation of alcohols. The nanohybrids Fe3O4@SiO2@PTMA, bearing catalytic TEMPO functionalities, were synthesized through distillation-precipitation polymerization (DPP) of the precursor monomer 2,2,6,6-tetramethyl-4-piperidyl methacrylate (TMPM) and subsequent oxidation reaction. TEM, FT-IR, DLS, EA confirmed and quantified the TEMPO loading of nanohydrids (1.0–2.4 mmol · g−1). It was found that the TEMPO loading, particle size, as well as surface hydrophilicity could be finely tuned via simply adjusting the TMPM monomer fraction during polymerization. The performance of the resultant nanohybrids as PIC was then evaluated in a typical Anelli system, which showed superior catalytic activity for selective oxidation of alcohols. Moreover, the PIC can be easily recycled by applying magnetic field, and reused for the following cycles of oxidation without any loss on either conversion or selectivity.



中文翻译:

新型高TEMPO负载磁性聚合物纳米杂化物:一种高效且可回收的Pickering界面催化剂

我们在这里报告了新型的磁聚合物纳米杂化物的设计和制备,该杂化物可用作醇的选择性氧化中的有效和可回收的Pickering界面催化剂(PIC)。通过前驱单体甲基丙烯酸2,2,6,6-四甲基-4-哌啶基酯(TMPM)的蒸馏-沉淀聚合(DPP)及其后续步骤,合成了具有催化TEMPO功能的纳米杂化Fe 3 O 4 @SiO 2 @PTMA。氧化反应。TEM,FT-IR,DLS,EA证实并定量了纳米氢化物(1.0–2.4 mmol·g -1)。已经发现,通过在聚合过程中简单地调节TMPM单体的比例,就可以对TEMPO的负载量,粒径和表面亲水性进行微调。然后在典型的Anelli系统中评估了所得纳米杂化物作为PIC的性能,该系统显示出对醇的选择性氧化具有优异的催化活性。此外,通过施加磁场,可以很容易地将PIC回收利用,并在随后的氧化循环中重新使用PIC,而不会降低转化率或选择性。

更新日期:2017-08-07
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