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首页> 外文期刊>Journal of Materials Science >Cu(II) complexes imobilized on functionalized mesoporous silica as catalysts for biomimetic oxidations
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Cu(II) complexes imobilized on functionalized mesoporous silica as catalysts for biomimetic oxidations

机译:固定在功能化介孔二氧化硅上的铜(II)配合物作为仿生氧化催化剂

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摘要

Mesoporous HMS silica was synthesized and functionalized with 3-aminopropyl-triethoxysilane (APTES) by a post-synthesis method. HMS and NH2-HMS supports were used for immobilization of two Cu(II) biomimetic complexes ([Cu(acac)(phen)(H2O)](ClO4), [Cu(acac)(Me(2)bipy)](ClO4)) or laccase enzyme. Mesoporous structure of the support; functionalization of silica surface, structure of ligands, and Cu complexes; and their immobilization were evidenced by XRD analysis, N-2 adsorption-desorption, SEM microscopy, TGA-DTA, IR and UV-Vis spectroscopy, and elemental analysis. The results confirm the structural integrity of the mesoporous hosts and successful anchoring of the metal complexes over the supports. For comparison, copper-substituted mesoporous silica (Cu-HMS) by using dodecylamine as structure-directing agent was also synthesized. All the synthesized materials were tested for their catalytic activity on the oxidation of 4-aminoantipyridine, 2,2'-azinobis (3-ethyl-benzothiazoline)-sulfonic acid (ABTS) with air, as well as in liquid phase oxidation of anisole and phenol with hydrogen peroxide. In order to verify the complex biomimetic activity, the Trametes versicolor laccase was immobilized by adsorption in the same supports.
机译:通过后合成方法合成了介孔HMS二氧化硅,并用3-氨基丙基-三乙氧基硅烷(APTES)将其官能化。 HMS和NH2-HMS支架用于固定两种仿铜复合物([Cu(acac)(phen)(H2O)](ClO4),[Cu(acac)(Me(2)bipy)](ClO4 )或漆酶。载体的介孔结构;二氧化硅表面的功能化,配体的结构和铜络合物; XRD分析,N-2吸附-解吸,SEM显微镜,TGA-DTA,IR和UV-Vis光谱以及元素分析证明了它们的固定性。结果证实了介孔主体的结构完整性以及金属络合物在载体上的成功锚固。为了比较,还合成了使用十二烷基胺作为结构导向剂的铜取代的介孔二氧化硅(Cu-HMS)。测试了所有合成材料在空气中对4-氨基抗吡啶,2,2'-叠氮双(3-乙基-苯并噻唑啉)-磺酸(ABTS)的氧化以及苯甲醚和苯甲醚的液相氧化的催化活性。苯酚与过氧化氢。为了验证复杂的仿生活性,通过吸附在相同的载体上固定了Trametes versicolor漆酶。

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