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Lignin Valorization by Cobalt-Catalyzed Fractionation of Lignocellulose to Yield Monophenolic Compounds
Stockholm University, Faculty of Science, Department of Organic Chemistry.
Stockholm University, Faculty of Science, Department of Organic Chemistry.
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Number of Authors: 62019 (English)In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 12, no 2, p. 404-408Article in journal (Refereed) Published
Abstract [en]

Herein, a catalytic reductive fractionation of lignocellulose is presented using a heterogeneous cobalt catalyst and formic acid or formate as a hydrogen donor. The catalytic reductive fractionation of untreated birch wood yields monophenolic compounds in up to 34 wt % yield of total lignin, which corresponds to 76% of the theoretical maximum yield. Model compound studies revealed that the main role of the cobalt catalyst is to stabilize the reactive intermediates formed during the organosolv pulping by transfer hydrogenation and hydrogenolysis reactions. Additionally, the cobalt catalyst is responsible for depolymerization reactions of lignin fragments through transfer hydrogenolysis reactions, which target the beta-O-4' bond. The catalyst could be recycled three times with only negligible decrease in efficiency, showing the robustness of the system.

Place, publisher, year, edition, pages
2019. Vol. 12, no 2, p. 404-408
Keywords [en]
biomass fractionation, birch wood, cobalt, heterogeneous catalysis, lignin, Green & Sustainable Science & Technology
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:su:diva-167685DOI: 10.1002/cssc.201802497ISI: 000459737500005PubMedID: 30485687OAI: oai:DiVA.org:su-167685DiVA, id: diva2:1301815
Available from: 2019-04-03 Created: 2019-04-03 Last updated: 2022-02-26Bibliographically approved
In thesis
1. Catalytic valorization of lignocellulose: Direct and sidestream upgrading approaches
Open this publication in new window or tab >>Catalytic valorization of lignocellulose: Direct and sidestream upgrading approaches
2021 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This work aims to explore different approaches for the valorization of lignocellulosic biomass. In this regard, two different strategies are presented: the catalytic upgrading of lignocellulose derivatives from industrial streams, such as pyrolytic oil and kraft lignin, and the direct catalytic fractionation of woody biomass. The first approach is explored in Paper I and II, while the second in Paper III and IV.

Different phenolic compounds were hydro-dearomatized using a heterogeneous catalytic system based on Pd/C and polymethylhydrosiloxane/H2O as a liquid hydrogen source. High yields of either cyclohexanones or cyclohexanols were achieved in high selectivity by varying the concentration of water. To prove the broad applicability of the method, commercially available bio-oils such as beechwood tar creosote and cardanol oil underwent hydrodearomatization using the developed catalytic systems (Paper I).

Kraft lignin, a byproduct of the paper manufacturing industry, has been valorized by steering its solubility properties through the production of a lipophilic lignin oil suitable for hydrotreatment. The enhanced solubility allowed its blending in common refinery carriers and full hydrodeoxygenation yielding hydrocarbons in the gasoline-diesel range. A particular focus was set on the mechanistic study of the esterification where a 13C labeling analysis was performed (Paper II).

Untreated birch wood was fractionated into its components while lignin was consequently depolymerized into monophenolic compounds. Cobalt was scrutinized to replace noble metals in reductive catalytic fractionation by synthetizing a heterogeneous catalyst supported on nitrogen-doped carbon. We found that adjusting the pH of the reaction medium affected the yields of the reaction. Under optimized conditions, monophenolic compounds could be obtained in up to 34 wt% yield relative to initial lignin. The role of the catalyst and reductants was investigated (Paper III).

The last chapter describes a pulping system able to parallelly perform the glucan purification and the catalytic upgrade of the lignin by-products while avoiding the contamination of the pulp with the heterogeneous catalyst. The system is based on a high-pressure Soxhlet combined with the ethanol-water organosolv, where Pd/C was selected as the heterogeneous catalyst. Using only CO2 as the acid source, lyocell grade dissolving pulp was produced in addition to lignin oil (Paper IV).

Place, publisher, year, edition, pages
Stockholm: Department of Organic Chemistry, Stockholm University, 2021. p. 65
Keywords
Lignin, biomass, catalytic fractionation, dearomatization, heterogeneous catalysis
National Category
Organic Chemistry
Research subject
Organic Chemistry
Identifiers
urn:nbn:se:su:diva-194071 (URN)978-91-7911-538-8 (ISBN)978-91-7911-539-5 (ISBN)
Public defence
2021-09-10, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 15:00 (English)
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Available from: 2021-08-18 Created: 2021-06-11 Last updated: 2022-02-25Bibliographically approved

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Rautiainen, SariDi Francesco, DavideTungasmita, Duangamol N.Samec, Joseph S. M.

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