4.6 Article

Bimetal Oxide Catalysts Selectively Catalyze Cellulose to Ethylene Glycol

Journal

JOURNAL OF PHYSICAL CHEMISTRY C
Volume 125, Issue 33, Pages 18170-18179

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c04446

Keywords

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Funding

  1. Foundation of Jiangsu Key Laboratory for Biomass Energy and Material [JSBEM202008]
  2. Opening Foundation of Chinese Academy of Sciences Key Laboratory for Biobased Materials and Chemicals [BMF-2020-03]
  3. Shandong Provincial Natural Science Foundation, China [ZR2019BC011]
  4. Opening Project of Shandong Eco-chemical Engineering Collaborative Innovation Center [XTCXQN14]
  5. Taishan Scholars Projects of Shandong [ts201511033]
  6. National Natural Science Foundation of China [21805158]
  7. 13th National 5-year R&D plans inrural areas [2016YFD0600804]
  8. Key R&D project of Shandong [2018GSF121031]

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This study successfully utilized a unique yolk-shell structured nanosphere catalyst to convert cellulose into ethylene glycol with high efficiency. Through structural and elemental analysis of the catalyst, it was found that tungsten and aluminum increased the acidity on the catalyst, resulting in higher selectivity of ethylene glycol.
Cellulose is an attractive and potential biomass material in nature. It has been studied for decades to convert it into high value-added chemical materials. In this article, we prepared a unique structure of a yolk-shell catalyst with uniform-sized Pd nanoparticles as the core and easily modified mesoporous silica as the shell, and the shell was modified by alumina and tungsten oxide. The modified Pd@W/Al-MSiO2 yolk-shell-structured nanosphere (YSNS) catalyst showed good catalytic activity in the conversion of cellulose to ethylene glycol: the conversion of cellulose was 96.1%, and the selectivity of ethylene glycol reached 56.5%. From XRD, XPS, and Al-27 MAS NMR spectral analysis, it can be seen that the existence of tungsten species would lead to the formation of more extra framework aluminum, which increased the acid strength; meanwhile, aluminum made the tungsten oxide oligomer increase, which increased the dispersion of tungsten species on the catalyst. The interaction of the two metal oxides increased the acidity and the increase in tungsten oxide oligomers were the reasons for the higher selectivity of ethylene glycol. Due to the protective effect of the shell on the Pd nanoparticles, there was no sintering and serious loss of Pd during the reaction, and only small amounts of tungsten and aluminum distributed in the pores and surface were lost. Therefore, the Pd@W/Al-MSiO2 YSNS catalyst maintained 48.5% ethylene glycol selectivity after five cycles.

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