Journal
ACS APPLIED NANO MATERIALS
Volume 5, Issue 8, Pages 11559-11566Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.2c02478
Keywords
lattice oxygen; reactive oxygen species; biomass transformation; amorphous catalyst; selective conversion
Funding
- National Natural Science Foundation of China [U1905215, 52072076]
- National Key Research and Development Program/Key Scientific Issues of Transformative Technology [2020YFA0710303]
- Fujian natural science foundation [2022J01554]
- key project of science and technology innovation of Fujian provincial department of education [2022G02002]
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The amorphous MnO2 nanostructure has been found to efficiently and selectively catalyze the aerobic oxidation of 5-hydroxymethylfurfural (HMF) to produce 2,5-furandicarboxylic acid (FDCA). It can also efficiently convert low-concentration 5-formyl-2-furancarboxylic acid (FFCA) intermediates into FDCA.
Aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) offers an appealing way to transform the biomass feedstock into chemical commodities but suffers from low efficiency and selectivity due to the formation of 5-formyl-2-furancarboxylic acid (FFCA) byproduct. Herein, we demonstrated that an amorphous MnO2 (amor-MnO2) nanostructure having a disordered lattice structure can carry O-L of high reactivity for catalyzing the aerobic oxidation of HMF to prepare FDCA efficiently and selectively. The FDCA formation rate of amor-MnO2 reaches up to 1307 mu mol(FDCA) g(cat)(-1) h(-1), about 8.2 times that of crystalline MnO2 (cry-MnO2) (160 mu mol(FDCA) g(cat)(-1) h(-1)) and surpassing many other state-of-the-art Mn-based catalysts. Kinetic studies reveal that the amor-MnO2 nanostructure can efficiently convert the low-concentration FFCA intermediate into FDCA, which helps tackle the rate-determining step in the HMF -> FFCA -> FDCA oxidation process. Density functional theory calculations and experimental measurements demonstrate that amor-MnO2 delivers superior lattice oxygen (O-L) activity and stronger O-2 adsorption capability when compared with the crystalline counterpart. The findings showcase the use of amorphous materials as advanced catalysts for achieving sustainable chemistry industry.
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