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Nb-Doping-Induced Transformation of Lewis and Brønsted Acidic Sites on Sulfonated TiO2 for Highly Efficient HMF Synthesis
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DOI：10.1021/acssuschemeng.4c10571.png)
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Abstract
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The presence and optimal balance of Lewis and Br & oslash;nsted acid sites in solid acid catalysts are crucial for their effectiveness in heterogeneous catalytic reactions. However, achieving this balance has proven to be a challenging task. In this study, the impact of niobium doping on sulfonated TiO2 catalysts was systematically discovered, both through theoretical modeling and experimental analysis. The introduction of Nb caused a shift in the proportion of Lewis and Br & oslash;nsted acid sites, resulting in a remarkable improvement in fructose conversion rates. Among the catalysts tested, the S-TiNb9 catalyst exhibited the highest reaction rate, achieving a conversion rate of 1.63 mMmin(-1), which is 9 times faster than that of TiO2 catalysts (0.19 mMmin(-1)). Detailed characterization techniques and density functional theory analysis revealed that the presence of Nb on the catalyst surface led to the formation of the Nb-SO4 structure, enhancing the acidity of Nb atoms rather than Ti-HSO4. This coexistence of Lewis and Br & oslash;nsted acidic sites facilitated an alternative pathway for fructose dehydration. The findings of this study represent a significant advancement in the field of acid catalysis by providing a straightforward and practical approach for creating highly efficient catalysts and alternative reaction pathways.
Keywords:
Lewis acid
Br & oslash
nsted acid
niobium doping
sulfonated TiO2 catalysts
HMF synthesis
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7.3
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1.7W
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10.7W
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