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固定在Fe3O4@SiO2介孔亚微球中的金属卟啉:用于烃类氧化的可重复使用的仿生催化剂。

Metalloporphyrins immobilized in Fe3O4@SiO2 mesoporous submicrospheres: Reusable biomimetic catalysts for hydrocarbon oxidation.

作者信息

Barbosa Isaltino A, de Sousa Filho Paulo C, da Silva Douglas L, Zanardi Fabrício B, Zanatta Lucas D, de Oliveira Adilson J A, Serra Osvaldo A, Iamamoto Yassuko

机构信息

Bioinorganic Chemistry and Rare Earth Laboratories, Department of Chemistry, Faculdade de Filosofia, Ciências e Letras de Ribeirão Preto, University of São Paulo, Av. Bandeirantes, 3900, 14040-901 Ribeirão Preto, SP, Brazil.

Department of Physics, Federal University of São Carlos, Av. Trabalhador São-Carlense, 400 - Pq. Arnold Schimidt, 13566-590 São Carlos, SP, Brazil.

出版信息

J Colloid Interface Sci. 2016 May 1;469:296-309. doi: 10.1016/j.jcis.2016.01.059. Epub 2016 Jan 27.

Abstract

We successfully immobilized metalloporphyrins (MeP) in mesoporous silica coating magnetite spheres. In this sense, we prepared two different classes of core@shell supports, which comprise aligned (Fe3O4-AM-MeP, MeP=FeP or MnP) and non-aligned (Fe3O4-NM-MeP, MeP=FeP or MnP) mesoporous magnetic structures. X-ray diffractometry and energy dispersive X-ray spectroscopy confirmed the mesoporous nature of the silica shell of the materials. Magnetization measurements, scanning and transmission electron microscopies (SEM/TEM), electrophoretic mobility (ζ-potential), and infrared spectroscopy (FTIR) also confirm the composition and structure of the materials. The catalysts maintained their catalytic activity during nine reaction cycles toward hydrocarbon oxidation processes without detectable catalyst leaching. The catalysis results revealed a biomimetic pattern of cytochrome P450-type enzymes, thus confirming that the prepared materials are can effectively mimic the activity of such groups.

摘要

我们成功地将金属卟啉(MeP)固定在介孔二氧化硅包覆的磁铁矿球中。从这个意义上说,我们制备了两类不同的核壳载体,它们包括排列有序的(Fe3O4-AM-MeP,MeP = FeP或MnP)和排列无序的(Fe3O4-NM-MeP,MeP = FeP或MnP)介孔磁性结构。X射线衍射和能量色散X射线光谱证实了材料二氧化硅壳的介孔性质。磁化测量、扫描和透射电子显微镜(SEM/TEM)、电泳迁移率(ζ电位)和红外光谱(FTIR)也证实了材料的组成和结构。在九个反应循环中,催化剂对烃氧化过程保持其催化活性,且未检测到催化剂浸出。催化结果揭示了细胞色素P450型酶的仿生模式,从而证实所制备的材料能够有效地模拟此类基团的活性。

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