Shanmugaraj Krishnamoorthy, Bustamante Tatiana M, Campos Cristian H, Torres Cecilia C
Departamento de Físico-Química, Facultad de Ciencias Químicas, Universidad de Concepción, Edmundo Larenas 129, Concepción 4070371, Chile.
Departamento de Química, Facultad de Ciencias Exactas, Universidad Andres Bello, Sede Concepción, Autopista Concepción-Talcahuano 7100, Talcahuano 4300866, Chile.
Materials (Basel). 2020 Feb 19;13(4):925. doi: 10.3390/ma13040925.
In this work, Au nanoparticles, supported in AlO nanowires (ANW) modified with (3-aminopropyl)trimethoxysilane were synthetized, for their use as catalysts in the hydrogenation reaction of 4-(2-fluoro-4-nitrophenyl)-morpholine and 4-(4-nitrophenyl)morpholin-3-one. ANW was obtained by hydrothermal techniques and the metal was incorporated by the reduction of the precursor with NaBH posterior to superficial modification. The catalysts were prepared at different metal loadings and were characterized by different techniques. The characterization revealed structured materials in the form of nanowires and a successful superficial modification. All catalysts show that Au is in a reduced state and the shape of the nanoparticles is spherical, with high metal dispersion and size distributions from 3.7 to 4.6 nm. The different systems supported in modified-ANW were active and selective in the hydrogenation reaction of both substrates, finding for all catalytic systems a selectivity of almost 100% to the aromatic amine. Catalytic data showed pseudo first-order kinetics with respect to the substrate for all experimental conditions used in this work. The solvent plays an important role in the activity and selectivity of the catalyst, where the highest efficiency and operational stability was achieved when ethanol was used as the solvent.
在本工作中,合成了负载于用(3-氨丙基)三甲氧基硅烷改性的AlO纳米线(ANW)中的金纳米颗粒,用于其在4-(2-氟-4-硝基苯基)吗啉和4-(4-硝基苯基)吗啉-3-酮氢化反应中的催化作用。ANW通过水热技术获得,并且在表面改性后通过用NaBH还原前驱体来引入金属。在不同的金属负载量下制备催化剂,并通过不同技术对其进行表征。表征揭示了纳米线形式的结构化材料以及成功的表面改性。所有催化剂均表明金处于还原态,纳米颗粒形状为球形,具有高金属分散性且尺寸分布在3.7至4.6nm之间。负载于改性ANW上的不同体系在两种底物的氢化反应中均具有活性和选择性,所有催化体系对芳胺的选择性几乎达到100%。催化数据表明,对于本工作中使用的所有实验条件,相对于底物呈现假一级动力学。溶剂在催化剂的活性和选择性中起重要作用,当使用乙醇作为溶剂时,可实现最高效率和操作稳定性。