Oxidation of 5-Hydroxymethylfurfural Using Ru Supported Mg-Fe Hydrotalcite Materials.

IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Peringayi Aswin, Rahul Gautham, Padinjare Purayil Neethu, Venkatachalam Ganesh, Shunmugavel Saravanamurugan, Ayyamperumal Sakthivel
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Abstract

A series of hydrotalcite-derived bimetallic catalysts were prepared, and Ru was loaded by wet impregnation. The catalyst retained a layered structure even after reduction, which was confirmed by Fourier-transform infrared spectroscopy and powder X-ray diffraction analyses. Among the prepared catalysts, ruthenium on magnesium-iron (Ru/MgFe) showed the best activity for 5-hydroxymethylfurfural oxidation under mild conditions in an aqueous medium (98.3% conversion at 120 °C, 3 h, and 30 bar O2), with the formation of 2, 5- furandicarboxylic acid (61.5%) as a major product along with 5-formyl 2-furancarboxylic acid and 2,5-diformylfuran as minor products. The highly dispersed metallic ruthenium on the surface of HT favored better activity. In addition, from the solvent studies, green solvent water showed higher activity than the other organic solvents. The activity of the catalyst reduced after the first cycle but regained upon treatment under a CO2 atmosphere, which facilitated the regeneration of surface basicity and hence helped in the reactivation of the catalyst. Overall, this work demonstrates that finely dispersed ruthenium on MgFe hydrotalcite (MgFe-HT) facilitates the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA). The Ru-dispersed MgFe-HT exhibits a high surface area (61.5 m2/g) along with surface basicity and redox properties, which contribute to a high HMF conversion (>99%) and a moderate FDCA yield (73.3%).

Ru负载Mg-Fe水滑石材料氧化5-羟甲基糠醛的研究
制备了一系列水滑石衍生的双金属催化剂,并采用湿浸渍法负载钌。通过傅里叶变换红外光谱和粉末x射线衍射分析,证实了催化剂在还原后仍保持层状结构。在所制备的催化剂中,钌对镁铁(Ru/MgFe)在温和条件下对5-羟甲基糠醛的氧化活性最好,在120℃,3 h, 30 bar O2条件下,转化率为98.3%,主要产物为2,5-呋喃二甲酸(61.5%),次要产物为5-甲酰基2-呋喃二甲酸和2,5-二甲酰呋喃。高温合金表面高度分散的金属钌具有较好的活性。此外,从溶剂研究来看,绿色溶剂水比其他有机溶剂表现出更高的活性。催化剂的活性在第一次循环后降低,但在CO2气氛下处理后恢复,这有助于表面碱度的再生,从而有助于催化剂的再活化。总的来说,这项工作表明,分散在MgFe水滑石(MgFe- ht)上的精细钌促进了5-羟甲基糠醛(HMF)氧化成2,5-呋喃二羧酸(FDCA)。钌分散的MgFe-HT具有高表面积(61.5 m2/g)、表面碱性和氧化还原性能,这有助于高HMF转化率(bb0 99%)和中等FDCA产率(73.3%)。
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来源期刊
Chemistry - An Asian Journal
Chemistry - An Asian Journal 化学-化学综合
CiteScore
7.00
自引率
2.40%
发文量
535
审稿时长
1.3 months
期刊介绍: Chemistry—An Asian Journal is an international high-impact journal for chemistry in its broadest sense. The journal covers all aspects of chemistry from biochemistry through organic and inorganic chemistry to physical chemistry, including interdisciplinary topics. Chemistry—An Asian Journal publishes Full Papers, Communications, and Focus Reviews. A professional editorial team headed by Dr. Theresa Kueckmann and an Editorial Board (headed by Professor Susumu Kitagawa) ensure the highest quality of the peer-review process, the contents and the production of the journal. Chemistry—An Asian Journal is published on behalf of the Asian Chemical Editorial Society (ACES), an association of numerous Asian chemical societies, and supported by the Gesellschaft Deutscher Chemiker (GDCh, German Chemical Society), ChemPubSoc Europe, and the Federation of Asian Chemical Societies (FACS).
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