Citation: Bin Guo, Lulu He, Gangfeng Tang, Li Zhang, Lin Ye, Bin Yue, Shik Chi Edman Tsang, Heyong He. Dehydration of sugars to 5-hydroxymethylfurfural and non-stoichiometric formic and levulinic acids over mesoporous Ta and Ta-W oxide solid acid catalysts[J]. Chinese Journal of Catalysis, ;2020, 41(8): 1248-1260. doi: S1872-2067(19)63519-9 shu

Dehydration of sugars to 5-hydroxymethylfurfural and non-stoichiometric formic and levulinic acids over mesoporous Ta and Ta-W oxide solid acid catalysts

Bin Guo ^a, ,
Lulu He ^a ,
Gangfeng Tang ^a ,
Li Zhang ^a ,
Lin Ye ^a ,
Bin Yue ^a ,
Shik Chi Edman Tsang ^b ,
Heyong He ^a

a Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials, Department of Chemistry, Fudan University, Shanghai 200433, China;
b Wolfson Catalysis Centre, Department of Chemistry, University of Oxford, Oxford OX1 3QR, UK

Received Date: 28 November 2019
Revised Date: 27 December 2019

Fund Project: This work was supported by the National Natural Science Foundation of China (21673046, 91645201).

A series of mesoporous Ta and Ta-W oxides have been prepared and employed as solid acid catalysts for the dehydration of fructose and glucose to 5-hydroxymethylfurfural (HMF). Solid state ³¹P MAS NMR spectroscopic results using trimethylphosphine (TMP) as a probe molecule show that the acid strength and the ratio of Brönsted to Lewis acid sites increase gradually with the addition of tungsten in tantalum oxide. It is found that high sugar conversion and HMF selectivity are achieved over catalyst with relatively high ratios of Brönsted to Lewis acid sites. Unexpected stoichiometric excess of formic acid relative to levulinic acid can be observed mainly because of direct decomposition of fructose over Lewis acid sites. The addition of 2-butanol leads to the increase of sugars conversion and the HMF selectivity, especially for the catalyst with high ratio of Brönsted to Lewis acid sites. Among them, Ta₇W₃ oxide catalyst shows 54% HMF selectivity and good reusability with the addition of 2-butanol by extracting HMF from aqueous phase and removing humins deposed on the surface of the catalyst.
- Glucose,
- Fructose,
- HMF,
- Solid acid,
- Tantalum oxide,
- Ta-W oxide
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