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Reductive lignocellulose fractionation into soluble lignin-derived phenolic monomers and dimers and processable carbohydrate pulps

(2015) ENERGY & ENVIRONMENTAL SCIENCE. 8(6). p.1748-1763
Author
Organization
Project
Biotechnology for a sustainable economy (Bio-Economy)
Abstract
A catalytic lignocellulose biorefinery process is presented, valorizing both polysaccharide and lignin components into a handful of chemicals. To that end, birch sawdust is efficiently delignified through simultaneous solvolysis and catalytic hydrogenolysis in the presence of a Ru on carbon catalyst (Ru/C) in methanol under a H-2 atmosphere at elevated temperature, resulting in a carbohydrate pulp and a lignin oil. The lignin oil yields above 50% of phenolic monomers (mainly 4-n-propylguaiacol and 4-n-propylsyringol) and about 20% of a set of phenolic dimers, relative to the original lignin content, next to phenolic oligomers. The structural features of the lignin monomers, dimers and oligomers were identified by a combination of GC/MS, GPC and 2D HSQC NMR techniques, showing interesting functionalities for forthcoming polymer applications. The effect of several key parameters like temperature, reaction time, wood particle size, reactor loading, catalyst reusability and the influence of solvent and gas were examined in view of the phenolic product yield, the degree of delignification and the sugar retention as a first assessment of the techno-economic feasibility of this biorefinery process. The separated carbohydrate pulp contains up to 92% of the initial polysaccharides, with a nearly quantitative retention of cellulose. Pulp valorization was demonstrated by its chemocatalytic conversion to sugar polyols, showing the multiple use of Ru/C, initially applied in the hydrogenolysis process. Various lignocellulosic substrates, including genetically modified lines of Arabidopsis thaliana, were finally processed in the hydrogenolytic biorefinery, indicating lignocellulose rich in syringyl-type lignin, as found in hardwoods, as the ideal feedstock for the production of chemicals.
Keywords
GAMMA-VALEROLACTONE, HETEROPOLY ACIDS, THERMOSETTING RESINS, MECHANOCATALYTIC DEPOLYMERIZATION, BIO-OIL, WHEAT-STRAW, KRAFT LIGNIN, RIGID POLYURETHANE FOAM, CATALYTIC CONVERSION, WOODY BIOMASS SOLIDS

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Citation

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Chicago
Van den Bosch, S, W Schutyser, Ruben Vanholme, T Driessen, SF Koelewijn, T Renders, Barbara De Meester, et al. 2015. “Reductive Lignocellulose Fractionation into Soluble Lignin-derived Phenolic Monomers and Dimers and Processable Carbohydrate Pulps.” Energy & Environmental Science 8 (6): 1748–1763.
APA
Van den Bosch, S., Schutyser, W., Vanholme, R., Driessen, T., Koelewijn, S., Renders, T., De Meester, B., et al. (2015). Reductive lignocellulose fractionation into soluble lignin-derived phenolic monomers and dimers and processable carbohydrate pulps. ENERGY & ENVIRONMENTAL SCIENCE, 8(6), 1748–1763.
Vancouver
1.
Van den Bosch S, Schutyser W, Vanholme R, Driessen T, Koelewijn S, Renders T, et al. Reductive lignocellulose fractionation into soluble lignin-derived phenolic monomers and dimers and processable carbohydrate pulps. ENERGY & ENVIRONMENTAL SCIENCE. 2015;8(6):1748–63.
MLA
Van den Bosch, S et al. “Reductive Lignocellulose Fractionation into Soluble Lignin-derived Phenolic Monomers and Dimers and Processable Carbohydrate Pulps.” ENERGY & ENVIRONMENTAL SCIENCE 8.6 (2015): 1748–1763. Print.
@article{6864310,
  abstract     = {A catalytic lignocellulose biorefinery process is presented, valorizing both polysaccharide and lignin components into a handful of chemicals. To that end, birch sawdust is efficiently delignified through simultaneous solvolysis and catalytic hydrogenolysis in the presence of a Ru on carbon catalyst (Ru/C) in methanol under a H-2 atmosphere at elevated temperature, resulting in a carbohydrate pulp and a lignin oil. The lignin oil yields above 50\% of phenolic monomers (mainly 4-n-propylguaiacol and 4-n-propylsyringol) and about 20\% of a set of phenolic dimers, relative to the original lignin content, next to phenolic oligomers. The structural features of the lignin monomers, dimers and oligomers were identified by a combination of GC/MS, GPC and 2D HSQC NMR techniques, showing interesting functionalities for forthcoming polymer applications. The effect of several key parameters like temperature, reaction time, wood particle size, reactor loading, catalyst reusability and the influence of solvent and gas were examined in view of the phenolic product yield, the degree of delignification and the sugar retention as a first assessment of the techno-economic feasibility of this biorefinery process. The separated carbohydrate pulp contains up to 92\% of the initial polysaccharides, with a nearly quantitative retention of cellulose. Pulp valorization was demonstrated by its chemocatalytic conversion to sugar polyols, showing the multiple use of Ru/C, initially applied in the hydrogenolysis process. Various lignocellulosic substrates, including genetically modified lines of Arabidopsis thaliana, were finally processed in the hydrogenolytic biorefinery, indicating lignocellulose rich in syringyl-type lignin, as found in hardwoods, as the ideal feedstock for the production of chemicals.},
  author       = {Van den Bosch, S and Schutyser, W and Vanholme, Ruben and Driessen, T and Koelewijn, SF and Renders, T and De Meester, Barbara and Huijgen, WJJ and Dehaen, W and Courtin, CM and Lagrain, B and Boerjan, Wout and Sels, BF},
  issn         = {1754-5692},
  journal      = {ENERGY \& ENVIRONMENTAL SCIENCE},
  language     = {eng},
  number       = {6},
  pages        = {1748--1763},
  title        = {Reductive lignocellulose fractionation into soluble lignin-derived phenolic monomers and dimers and processable carbohydrate pulps},
  url          = {http://dx.doi.org/10.1039/c5ee00204d},
  volume       = {8},
  year         = {2015},
}

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