Aerobic Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid over Holey 2 D Mn2O3 Nanoflakes from a Mn-based MOF

被引:81
|
作者
Bao, Liwei [1 ]
Sun, Fang-Zhou [1 ]
Zhang, Guo-Ying [2 ,3 ]
Hu, Tong-Liang [1 ,4 ]
机构
[1] Nankai Univ, Natl Inst Adv Mat, Sch Mat Sci & Engn, Tianjin Key Lab Met & Mol Based Mat Chem, Tianjin 300350, Peoples R China
[2] Tianjin Normal Univ, Coll Chem, Key Lab Inorgan Organ Hybrid Funct Mat Chem, Minist Educ, Tianjin 300387, Peoples R China
[3] Shandong Normal Univ, Shandong Prov Key Lab Clean Prod Fine Chem, Jinan 250014, Shandong, Peoples R China
[4] Nankai Univ, Tianjin Key Lab Rare Earth Mat & Applicat, Key Lab Adv Energy Mat Chem, Minist Educ, Tianjin 300071, Peoples R China
关键词
aerobic oxidation; biomass; heterogeneous catalysis; manganese; metal-organic frameworks; METAL-ORGANIC FRAMEWORK; SELECTIVE OXIDATION; OXYGEN REDUCTION; MANGANESE OXIDES; MIXED OXIDES; QUASI-MOF; BIOMASS; NANOPARTICLES; ENERGY; CARBON;
D O I
10.1002/cssc.201903018
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), a promising renewable monomer to produce bio-based polymers such as polyethylene furanoate (PEF), has recently emerged as the subject of increasing interest. Here, holey 2 D Mn2O3 nanoflakes were obtained by a facile thermal treatment of a Mn-based metal-organic framework (MOF) precursor. The structural and morphological properties of the nanoflakes were characterized by powder XRD, FTIR, SEM and TEM to explore the formation process. It was inferred that the linker loss in the MOF precursor and the oxidation of the Mn cation induced by the heat-treatment in air were responsible for the formation of holey 2 D Mn2O3 nanoflakes. The specific morphology and redox cycle of the Mn cation on the surface endowed the synthesized nanoflakes with promising performance on the selective oxidation. The obtained nanoflakes calcined at 400 degrees C (M400) afforded over 99.5 % yield of FDCA at complete conversion of HMF, which is superior to the catalytic activity of commercial Mn2O3 and activated MnO2. To our knowledge, Mn2O3 exhibiting such a high performance on the aerobic oxidation of HMF to FDCA has not yet been reported. Based on the investigation of the experimental parameters, a plausible reaction mechanism was proposed.
引用
收藏
页码:548 / 555
页数:8
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