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Tandem catalysis of furfural to γ-valerolactone over polyoxometalate-based metal-organic frameworks: Exploring the role of confinement in the catalytic process

Author

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  • Ma, Mingwei
  • Hou, Pan
  • Zhang, Peng
  • Guo, Qi
  • Yue, Huijuan
  • Huang, Jiahui
  • Tian, Ge
  • Feng, Shouhua

Abstract

Polyoxometalate-based metal-organic frameworks (POMOFs) with bifunctional Lewis-Brønsted acid were designed by confining polyoxometalates (POMs: phosphotungstic acid (PW), phosphomolybdic acid (PMo) or silicotungstic acid (SiW)) within the Zr-MOFs. The confined POMs not only have their own Brønsted acid, but can also regulate the Lewis acid strength of the POMOFs via charge regulation, ultimately allowing the POMOFs to display superior catalytic performance in the tandem catalysis of furfural (FAL) to γ-valerolactone (GVL). Among the three catalysts (POMOF-PW, POMOF-PMo and POMOF-SiW), a complete conversion of FAL was achieved, while POMOF-PW exhibited the highest GVL yield (58.1 %) at 160 °C within 23 h. The leaching experiment and structural characterization of the catalyst before and after recycling confirmed the stability of the catalyst structure. The humin originates from the polymerization of furan ring-containing compounds driven by Brønsted acid. The adsorption configuration of the substrate molecules on the catalyst offers a new explanation for the tandem reaction process, i.e. that perpendicular adsorption performs only the first step of the tandem reaction, while the coexistence of perpendicular and horizontal adsorption permits the entire reaction process. This work gives unique insights into the tandem reaction of FAL and can guide the design of efficient tandem reaction catalysts.

Suggested Citation

  • Ma, Mingwei & Hou, Pan & Zhang, Peng & Guo, Qi & Yue, Huijuan & Huang, Jiahui & Tian, Ge & Feng, Shouhua, 2024. "Tandem catalysis of furfural to γ-valerolactone over polyoxometalate-based metal-organic frameworks: Exploring the role of confinement in the catalytic process," Renewable Energy, Elsevier, vol. 227(C).
    • Handle: RePEc:eee:renene:v:227:y:2024:i:c:s0960148124005391
    DOI: 10.1016/j.renene.2024.120474
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    References listed on IDEAS

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    1. Li, Mengzhu & Wei, Junnan & Yan, Guihua & Liu, Huai & Tang, Xing & Sun, Yong & Zeng, Xianhai & Lei, Tingzhou & Lin, Lu, 2020. "Cascade conversion of furfural to fuel bioadditive ethyl levulinate over bifunctional zirconium-based catalysts," Renewable Energy, Elsevier, vol. 147(P1), pages 916-923.
    2. Yan, Puxiang & Wang, Haiyong & Liao, Yuhe & Wang, Chenguang, 2023. "Zeolite catalysts for the valorization of biomass into platform compounds and biochemicals/biofuels: A review," Renewable and Sustainable Energy Reviews, Elsevier, vol. 178(C).
    3. Xiang, Wenlong & Ren, Jie & Chen, Si & Shen, Chenyang & Chen, Yifei & Zhang, Minhua & Liu, Chang-jun, 2020. "The metal–organic framework UiO-66 with missing-linker defects: A highly active catalyst for carbon dioxide cycloaddition," Applied Energy, Elsevier, vol. 277(C).
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