Abstract

The conversion of cellulose into ethylene glycol remains a significant challenge in the biobased domain. Here we explored the activity of various bulk and mesoporous (doped) tungsten oxides in combination with carbon-supported ruthenium for obtaining ethylene glycol from cellulose. Tungstite and sub-stoichiometric tungsten oxides are more active and selective than monoclinic WO3. Doping tungstite with early transition metals enhanced the rate of cellulose depolymerization to glucose through a higher Brønsted acidity, although this did not improve the overall performance as the higher acidity resulted in a higher rate of humin formation. The increased acidity of mesoporous sub-stoichiometric tungsten oxide compared to tungstite had a similar adverse effect. Doping this material with niobium improved ethylene glycol selectivity at similar conversion. Kinetic studies showed that the majority of ethylene glycol is produced in the first hour for three optimized catalysts, with undoped bulk tungstite being the most efficient catalytic material. Impregnation of these materials with ruthenium instead of using carbon-supported ruthenium as a co-catalyst was most beneficial for tungstite, as it showed improved ethylene glycol selectivity and lower polyol yields after 1 h of reaction time.

Highlights

  • Ethylene glycol (EG) is an important chemical, which is mainly used for anti-freeze purposes and as a raw material for the production of polyester fibers [1]

  • We explored the activity of various bulk and mesoporous tungsten oxides in tandem with carbon-supported ruthenium for cellulose conversion into EG

  • We investigated the influence of doping tungstite and mesoporous tungsten oxides with early transition metals on the depolymerization of cellulose to glucose and the retro-aldolization of glucose to C2 aldehydes

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Summary

Introduction

Ethylene glycol (EG) is an important chemical, which is mainly used for anti-freeze purposes and as a raw material for the production of polyester fibers [1]. The occurring reactions can be classified into cellulose hydrolysis, retro-aldolization of glucose and other saccharides, hydrogenation of aldehydes and ketones, and dehydration of polyols and hydrogenation of the resulting C]C bonds. Our earlier investigation on glucose valorization to 5-hydroxymethylfurfural demonstrated that (doped) tungstite (WO3.H2O) and sub-stoichiometric tungsten oxides are significantly more active compared to monoclinic WO3 [20]. We tested these materials using ruthenium as a hydrogenation co-catalyst, both supported on carbon and directly impregnated on our catalysts. We explored the activity of various bulk and mesoporous (doped) tungsten oxides in tandem with carbon-supported ruthenium for cellulose conversion into EG. We optimized the ruthenium loading towards optimum EG yield

Chemicals
Catalyst preparation
Characterization
Catalytic activity tests
Product analysis
Findings
Conclusion
Full Text
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