Abstract
Developing cost-effective processing strategies for the preparation of fuel-precursor chemicals, including 5-hydroxymethylfurfural (HMF) and furfural, has been dedicatedly researched over the last few years. These compounds are typically produced using different carbohydrate sources, say furfural using xylose and HMF using glucose. Herein, we report the significant formation of both these furfurals using a single glucose source over the fine-tuned Fe2+@SO3-CD nanocomposite. The catalyst exhibiting two different acidic sites, such as Lewis and Brønsted, developed by the iron (II) metal and sulfonate groups, respectively, offered a synergistic effect on the glucose decomposition into furfurals. Mechanistically, the iron (II) Lewis metal acid sites play a vital role in the significant formation of furfurals. Furthermore, the THF/H2O biphasic system influenced a selective formation of HMF and furfural, achieving as high as 85% HMF (94% selectivity) in 1:2 THF/H2O and 56% furfural (90% selectivity) in 1:1 THF/H2O. The recyclability study showed that the catalyst is effective for 4 cycles. The green metrics analysis of the solid acid catalysis represented a greener strategy for furfurals production. Overall, the catalytic setup can be upscaled because of the involvement of cheaper precursors and less labor-intensive catalyst preparation.
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Acknowledgements
The authors thank the Department of Biotechnology (DBT) for the financial support for this work through the flagship program (Grant no. BT/CIAB-Flagship/2018). GJ thanks the Department of Science and Technology (DST) for the project grant (No. SB/S2/RJN-047/2015) and DST-SERB for the Ramanujan Fellowship.
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Raina Sharma contributed to methodology, validation, investigation and writing including review and editing; Abdul Selim performed investigation and writing including review and editing; Bhawana Devi, Senthil M Arumugam, and Shaifali Sartaliya carried out investigation; Sasikumar Elumalai performed supervision and writing including review and editing; Govindasamy Jayamurugan contributed to conceptualization, supervision, writing of the original draft, and writing including review and editing.
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The early version of the manuscript is available at the ChemRxiv non-peer review platform at https://doi.org/10.26434/chemrxiv-2022-lx28n. The authors declare no competing financial interest.
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Supplementary file1 (PDF 1369 KB) The supplementary information (SI) provides additional details on the catalyst’s analytical characterization (UV-vis spectra, AFM, TGA, TPD, FE-SEM/EDX and relative abundance, elemental mapping, and HPLC data), recycle performance with P-XRD and TGA data, green metrics parameter formulae, and control study and literature comparison tables
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Sharma, R., Selim, A., Devi, B. et al. Realizing direct conversion of glucose to furfurals with tunable selectivity utilizing a carbon dot catalyst with dual acids controlled by a biphasic medium. Biomass Conv. Bioref. 14, 11445–11457 (2024). https://doi.org/10.1007/s13399-022-03182-w
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DOI: https://doi.org/10.1007/s13399-022-03182-w