Depolymerization of Technical Lignins in Supercritical Ethanol: Effects of Lignin Structure and Catalyst
| Autor: | Roger Gadiou, Loïc Vidal, Yann Le Brech, Frederique Bertaud, Jean-Marc Le Meins, Sébastien Leclerc, Erika Bartolomei, Anthony Dufour |
|---|---|
| Přispěvatelé: | Laboratoire Réactions et Génie des Procédés (LRGP), Centre National de la Recherche Scientifique (CNRS)-Université de Lorraine (UL), Institut de Science des Matériaux de Mulhouse (IS2M), Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Centre Technique du Papier (CTP), Laboratoire Énergies et Mécanique Théorique et Appliquée (LEMTA ), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), ANR-16-CE06-0007,PhenoLiq,Production de composés Phénoliques par Liquéfaction de la lignine(2016), Leclerc, Sebastien, Production de composés Phénoliques par Liquéfaction de la lignine - - PhenoLiq2016 - ANR-16-CE06-0007 - AAPG2016 - VALID |
| Jazyk: | angličtina |
| Rok vydání: | 2021 |
| Předmět: |
Ethanol
[SPI.GPROC] Engineering Sciences [physics]/Chemical and Process Engineering Depolymerization General Chemical Engineering Energy Engineering and Power Technology 02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Supercritical fluid 0104 chemical sciences Catalysis [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry chemistry.chemical_compound Fuel Technology chemistry Chemical engineering Lignin [SPI.GPROC]Engineering Sciences [physics]/Chemical and Process Engineering 0210 nano-technology |
| Zdroj: | Energy & Fuels Energy & Fuels, American Chemical Society, 2021, 35 (21), pp.17769-17783. ⟨10.1021/acs.energyfuels.1c02704⟩ Energy & Fuels, 2021, 35 (21), pp.17769-17783. ⟨10.1021/acs.energyfuels.1c02704⟩ |
| ISSN: | 0887-0624 1520-5029 |
| DOI: | 10.1021/acs.energyfuels.1c02704⟩ |
| Popis: | International audience; Three complementary Kraft lignins and a Soda lignin were characterized by NMR (31P, 13C, and HSQC) and GPC. Their theoretical yield in monomers (TMY) assuming a complete cleavage of all β-O-4 linkages was calculated based on these analyses. The most recalcitrant Kraft lignin according to the TMY criteria was depolymerized in supercritical ethanol (250 °C, H2, 110 bar) with Pt/C, Ni/C, and Ru/C catalysts. All catalysts present an important effect on monomers (analyzed by GC/MS), oligomers (by UV fluorescence), and char yields. They promote cracking reactions and the stabilization of the broken bonds by H-transfers. The hydrogenation of the side chains of the monomers is also promoted to notably produce propyl-guaiacol. We show that an oligomeric pool prevails for all catalysts. Then, the effect of lignin structure on the depolymerization mechanism was studied by comparing the 4 lignins with the least precious catalyst (Ni/C). The S/G ratio of monomers is well related to the S/G ratio of lignins. Under our conditions, the β-O-4 content and the TMY do not control the yields in monomers. They are not relevant indicators for the depolymerization of these recalcitrant technical lignins. Future work should focus on novel catalysts and processes to improve the selective conversion of C–C bonds if monomers remain the targeted product. |
| Databáze: | OpenAIRE |
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