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5-Hydroxymethylfurfural catalytic oxidation under mild conditions by Co (II), Fe (III) and Cu (II) Salen complexes supported on SBA-15: Synthesis, characterization and activity
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2017-09-01 , DOI: 10.1016/j.apcata.2017.08.035
Daniela Xulú Martínez-Vargas , Javier Rivera De La Rosa , Ladislao Sandoval-Rangel , Jorge Luis Guzmán-Mar , Marco A. Garza-Navarro , Carlos J. Lucio-Ortiz , David A. De Haro-Del Río

In the present work, an alternative system of 5-hydroxymethylfurfural (HMF) oxidation was studied, in an effort to avoid the use of expensive precious metal catalysts, high pressures and systems not environmentally friendly. The catalysts tested were Co (II), Fe (II) and Cu (II) Salen complexes supported on SBA-15 (Co Salen/SBA-15, Fe Salen/SBA-15 and Cu Salen/SBA-15 respectively). The reaction was carried out in aqueous medium at room temperature (25 °C ± 1) and atmospheric pressure, using hydrogen peroxide (H2O2) as the only oxidant agent. The effect of various reaction conditions such as H2O2 content, oxidant agent amount, different transition metals present in the catalyst and temperature were evaluated. The HMF and the reaction products such as; 2,5-diformylfuran (DFF), 2,5-furandicarboxylic acid (FDCA), 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) and 5-formyl-2-furancarboxylic acid (FFCA) were followed by high performance liquid chromatography (HPLC) measurements. The selectivity and reaction kinetics under different reaction conditions was studied. The different synthesized catalysts were extensively characterized by UV–vis spectroscopy, subsequently by FTIR, DR-UV–vis, AA and XPS spectroscopy and through nitrogen physorption, which was related to its catalytic activity. The successful synthesis of SBA-15 support was confirmed by its textural properties and STEM. From the experimental data obtained a reaction mechanism with parallel reactions was proposed founding that the oxidation route of the alcohol group in HMF is favored over of the oxidation of the aldehyde group on the other side of the molecule.



中文翻译:

在SBA-15上负载的Co(II),Fe(III)和Cu(II)Salen配合物在温和条件下对5-羟甲基糠醛进行催化氧化:合成,表征和活性

在目前的工作中,研究了5-羟甲基糠醛(HMF)氧化的替代系统,以努力避免使用昂贵的贵金属催化剂,高压和不环保的系统。测试的催化剂为负载在SBA-15上的Co(II),Fe(II)和Cu(II)Salen配合物(分别为Co Salen / SBA-15,Fe Salen / SBA-15和Cu Salen / SBA-15)。反应在水介质中于室温(25°C±1)和大气压下进行,使用过氧化氢(H 2 O 2)作为唯一的氧化剂。H 2 O 2等各种反应条件的影响含量,氧化剂量,催化剂中存在的不同过渡金属和温度进行了评估。HMF和反应产物,如;2,5-二甲酰基呋喃(DFF),2,5-呋喃二甲酸(FDCA),5-羟甲基-2-呋喃甲酸(HMFCA)和5-甲酰基-2-呋喃甲酸(FFCA)之后进行高效液相色谱( HPLC)测量。研究了不同反应条件下的选择性和反应动力学。不同的合成催化剂通过紫外可见光谱,随后的FTIR,DR-UV可见光谱,AA和XPS光谱以及通过氮吸收法进行了广泛表征,这与其催化活性有关。SBA-15载体的成功合成被其质地特性和STEM证实。

更新日期:2017-09-01
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