期刊
JOURNAL OF ENERGY CHEMISTRY
卷 62, 期 -, 页码 599-609出版社
ELSEVIER
DOI: 10.1016/j.jechem.2021.04.022
关键词
5-Hydroxymethylfurfural; Aerobic oxidation; 2,5-Furandicarboxylic acid; Bifunctional Au/Mg-Beta catalyst; Structural reconstruction
资金
- National Natural Science Foundation of China [22072126, 22002133, 21676230, 21373177]
- Natural Science Foundation of Shandong Province [ZR2020QB055]
- Young Scholars Research Fund of Yantai University [HY19B26]
The study focuses on the performance of Au catalysts supported by Mg-Beta zeolites in the oxidation of biomass-derived 5-hydroxymethylfurfural to FDCA, showing that the support structure significantly affects the yield, with strong basicity of Mg-Beta zeolites not only improving the yield but also reducing the amount of additional base required.
The selective aerobic oxidation of biomass-derived 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid (FDCA, a potential renewable substitution of fossil-based terephthalic acid to produce polyethylene 2,5-furandicarboxylate plastic) is an appealing transformation for constructing eco-friendly and sustainable chemical processes. Au supported catalysts have showed encouraging performances for this well-received conversion, whose catalytic behavior was greatly affected by the adopted support derived from the existence of metal-support interactions. Herein, a series of Mg-Beta zeolites were hydrothermally synthesized via developed structural reconstruction, which were employed as basic supports for Au catalysts to construct bifunctional catalysts. The relationship between structure (Au particle size, basicity within zeolites and Au delta+ contents) and FDCA yield was concretely established. The conclusion was made that the utilization of Mg-Beta zeolites with strong basicity as the support could not only improve the FDCA yield but also decrease the amount of additional base. Furthermore, the possible reaction mechanism was also proposed via tracking time-dependent variations of corresponding organics and controlled experiment. This work provides some guidance for rationally designing multifunctional catalysts in the view of integrating metal catalysts with metallosilicate zeolites, which was beneficial to the catalytic upgrading of organic compounds with multiple functional groups. (C) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
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