Abstract
In this work, we developed an approach of one-pot complete catalytic conversion of woody biomass into two value product streams: lignin-derived aromatics (monomer yield of 68.54% and oligomer yield of 29.65% based on lignin mass) and (semi-)cellulose-derived small molecular alcohols (about 59.60% of biomass mass). These could be afforded by conducting lignocellulose depolymerization over metal-alkaline catalysts in a mixed n-butanol/H2O solvent system at 250 °C and 30 bar H2. In the valorization process, the homogenous mixture of n-butanol-H2O solvents extract and depolymerize both lignin and hemicellulose, while the catalysts and H2 are essential to cleave the inter-/intramolecular linkage of lignocellulose into target products. After the reaction, the phase separation of n-butanol and H2O takes place when system temperature drops below 125 °C, providing a mild and effective strategy to isolate lignin-derived aromatics (n-butanol phase) from small molecular alcohols/acids (aqueous phase). Ru/C and alkali catalysts are collected by filtration from n-butanol phase and H2O phase, respectively. Meanwhile, the effect of metal-alkali coupled catalysts facilitates the cleavage of β-O-4 linkage of lignin and increases the attainability of (semi-)cellulose-derived oligomers and the small molecular alcohols. This catalytic system provides a versatile valorization approach for biomass catalysis to bio-based chemicals.
Highlights
With the increasing demand of global energy and the declining of crude oil attainability as fuel, chemicals and energy [1], the proportion of energy and chemicals provided by renewable resources is gradually increasing and becoming an increasingly important resource for the sustainable production of fuels and chemicals [2,3]
3.1 Ru/C cooperated with MgO for catalytic valorization lignocellulose
Much soluble carbohydrate products increase with the mass of oligomers increasing and monomers decreasing when the hydrogen pressure increases from 10 bar to 40 bar, indicating that high H2 pressure facilitates the cleavage of intermolecular linkages between lignin and cellulose/hemicellulose
Summary
With the increasing demand of global energy and the declining of crude oil attainability as fuel, chemicals and energy [1], the proportion of energy and chemicals provided by renewable resources (such as biomass) is gradually increasing and becoming an increasingly important resource for the sustainable production of fuels and chemicals [2,3]. Biomass serves as a natural renewable chemical resources that can be converted to high added-value products [12,13,14]. Due to the great difference of lignin and (semi-cellulose) structures, the final depolymerized products derived one-pot conversion of biomass are too complex and quite different, product separation is necessary for upgrading or utilization after the end of the reaction. We developed and investigated a catalytic valorization route, targeting the one-step conversion of woody biomass and separation into two sets of value products: (i) lignin derived aromatics, (ii) (semi-)cellulose-derived small molecular (C2~C5) alcohols and acids (Fig.). Which is reduced the difficulty of the product separation and production cost in one-pot complete dissolution polymerization system
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