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Heterogeneous Catalysts for Lignin Upgrading
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Heterogeneous Catalysts for Lignin Upgrading

A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Environmental Catalysis".

Deadline for manuscript submissions: closed (31 January 2022) | Viewed by 12777

Special Issue Editor

Dr. Laurent Djakovitch

E-Mail Website1 Website2
Guest Editor
Institut de Recherches sur la Catalyse, 2 avenue Albert Einstein, 69626 Villeurbanne Cedex, France
Interests: Environmental Science; Chemistry; Chemical Engineering; Materials Science; Biochemistry; Genetics and Molecular Biology
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear colleagues,

Lignin valorization became last years a highly attractive area due to its potential for producing chemicals, fuels and bio-based materials, particularly with high content of aromatics. Actually, lignin is the second most abundant bio-polymer that did not compete with food industries, after cellulose, representing ca. 25% of available biomass and the only one made of aromatics. Lignin are mainly produced by paper industries (i.e.: Kraft, Sulfite or Soda processes); however, few new biorefineries produce as well so called Organosolv lignin. If lignin valorization to energy is somewhat addressed in the paper industries through burning, lignin upgrading to chemical, with high added-value, stay in its infancy. Therefore, developing efficient processes to produce aromatics from lignin remains a major challenge justifying the intensive researches in this area. Theses researches aim also at enhancing the economical balance of biorefineries.

With this mind, the development of catalysts, mainly heterogeneous catalysts, represent a very attractive area. When associated to processes, these researches represent therefore key investigations for developing further biorefineries by defining breakthrough technologies for the chemical industries.

It is a pleasure to invite you to contribute to this special issue of Catalysts given your intensive contributions to this area. This special issue covers development of catalysts (heterogeneous and homogeneous systems), processes through design and use of reactor including engineering aspects, industrial applications from demonstration plants to production implementations.  

Original research papers, as well as review articles are welcome. While focused on development and use of heterogeneous catalysts to upgrade lignin to chemical, researches devoted to discovery of efficient homogeneous systems are also strongly encouraged.

Dr. Laurent Djakovitch
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Catalysts is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Lignin
  • Chemicals
  • Biomass upgrading
  • Catalysis
  • Heterogeneous catalysts
  • Chemical engineering
  • Processes
  • Biorefinery

Published Papers (5 papers)

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Research

18 pages, 4260 KiB  
Communication
Solvent Effect in Catalytic Lignin Hydrogenolysis
by Dennis Panke, German Bechthold and Thomas E. Müller
Catalysts 2022, 12(6), 664; https://doi.org/10.3390/catal12060664 - 17 Jun 2022
Cited by 2 | Viewed by 2294
Abstract
The solvent effect in the catalytic depolymerization of the three-dimensional network of lignin is discussed based on recent reports in this field. Also, the results of an experimental study on the depolymerization of kraft lignin are presented. The cleavage of ether bonds within [...] Read more.
The solvent effect in the catalytic depolymerization of the three-dimensional network of lignin is discussed based on recent reports in this field. Also, the results of an experimental study on the depolymerization of kraft lignin are presented. The cleavage of ether bonds within the lignin network was promoted using ruthenium and platinum on activated carbon (Ru/C and Pt/C), two common hydrogenolysis catalysts. Methanol was identified as a suitable solvent. Noteworthy, under the chosen reaction conditions, the catalysts showed significant resilience to the sulfur present in kraft lignin. The conversion of kraft lignin to lignin oil was strongly affected by the reaction conditions. Although the Ru/C catalyst provided the highest yield at supercritical conditions, a maximum yield was obtained for the Pt/C catalyst at near-critical conditions. The formation of guaiacol, 4-alkylguaiacols, isoeugenol, and 4-ethyl-2,6-dimethoxyphenol is attributed to the solubility of oligomeric lignin fragments in the solvent and the relative propensity of specific groups to adsorb on the catalyst surface. Full article
(This article belongs to the Special Issue Heterogeneous Catalysts for Lignin Upgrading)
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20 pages, 5223 KiB  
Article
Investigating (Pseudo)-Heterogeneous Pd-Catalysts for Kraft Lignin Depolymerization under Mild Aqueous Basic Conditions
by Dolorès Bourbiaux, Yu Xu, Laurence Burel, Firat Goc, Pascal Fongarland, Régis Philippe, Guillaume Aubert, Cyril Aymonier, Franck Rataboul and Laurent Djakovitch
Catalysts 2021, 11(11), 1311; https://doi.org/10.3390/catal11111311 - 29 Oct 2021
Cited by 8 | Viewed by 1731
Abstract
Lignin is one of the main components of lignocellulosic biomass and corresponds to the first renewable source of aromatic compounds. It is obtained as a by-product in 100 million tons per year, mainly from the paper industry, from which only 2–3% is upgraded [...] Read more.
Lignin is one of the main components of lignocellulosic biomass and corresponds to the first renewable source of aromatic compounds. It is obtained as a by-product in 100 million tons per year, mainly from the paper industry, from which only 2–3% is upgraded for chemistry purposes, with the rest being used as an energy source. The richness of the functional groups in lignin makes it an attractive precursor for a wide variety of aromatic compounds. With this aim, we investigated the Pd-catalyzed depolymerization of lignin under mild oxidizing conditions (air, 150 °C, and aqueous NaOH) producing oxygenated aromatic compounds, such as vanillin, vanillic acid, and acetovanillone. Palladium catalysts were implemented following different strategies, involving nanoparticles stabilized in water, and nanoparticles were supported on TiO2. Significant conversion of lignin was observed in all cases; however, depending on the catalyst nature and the synthetic methods, differences were observed in terms of selectivity in aromatic monomers, mainly vanillin. All these aspects are discussed in detail in this report, which also provides new insights into the role that Pd-catalysts can play for the lignin depolymerization mechanism. Full article
(This article belongs to the Special Issue Heterogeneous Catalysts for Lignin Upgrading)
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21 pages, 2880 KiB  
Article
Selective C–C Bond Cleavage in Diols and Lignin Models: High-Throughput Screening of Metal Oxide-Anchored Vanadium in Mesoporous Silica
by Xinnan Lu, Roxanne Clément, Yong Lu, Belén Albela, R. Tom Baker and Laurent Bonneviot
Catalysts 2021, 11(8), 901; https://doi.org/10.3390/catal11080901 - 26 Jul 2021
Cited by 2 | Viewed by 2609
Abstract
The development of selective and robust heterogeneous oxidation catalysts is an enabling technology for conversion of biomass-derived platform chemicals. Vanadium active sites were incorporated into the structure of mesoporous silica via an ultra-fast, one-pot synthesis method based on microwave-assisted heating. In addition, Al/Ti/Zr/Ce [...] Read more.
The development of selective and robust heterogeneous oxidation catalysts is an enabling technology for conversion of biomass-derived platform chemicals. Vanadium active sites were incorporated into the structure of mesoporous silica via an ultra-fast, one-pot synthesis method based on microwave-assisted heating. In addition, Al/Ti/Zr/Ce anchoring ions were introduced in order to minimize vanadium leaching and better control its dispersion. The supported V-(Al/Ti/Zr/Ce)-MCM-41 composite materials were assessed as catalysts for aerobic C–C bond cleavage of simple models for lignin (1,2-diphenyl-2-methoxyethanol) and sugar-derived polyalcohols (meso-hydrobenzoin). The TiIV ions proved to be the best anchors to prevent V leaching, while AlIII and ZrIV ions were the best to improve selective conversion of the substrates. The active sites in these catalysts are shown to be 2D VOx layers stabilized on the anchors. In a screen of twelve solvents, weakly polar solvents like toluene were found to be most suitable for this reaction, as was environmentally friendly ethyl acetate. The above properties, together with the high selectivity for C–C bond cleavage, advocate for a heterogeneous catalytic pathway, intrinsically different from that reported previously for molecular oxovanadium (V) catalysts. Full article
(This article belongs to the Special Issue Heterogeneous Catalysts for Lignin Upgrading)
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27 pages, 16203 KiB  
Article
Catalytic Liquefaction of Kraft Lignin with Solvothermal Approach
by Woldemichael Sebhat, Ayman El Roz, Pascal Fongarland, Léa Vilcocq and Laurent Djakovitch
Catalysts 2021, 11(8), 875; https://doi.org/10.3390/catal11080875 - 21 Jul 2021
Cited by 10 | Viewed by 2186
Abstract
Lignin is a natural biopolymer present in lignocellulosic biomass. During paper pulp production with the Kraft process, it is solubilized and degraded in Kraft lignin and then burned to recover energy. In this paper, the solvolysis of Kraft lignin was studied in water [...] Read more.
Lignin is a natural biopolymer present in lignocellulosic biomass. During paper pulp production with the Kraft process, it is solubilized and degraded in Kraft lignin and then burned to recover energy. In this paper, the solvolysis of Kraft lignin was studied in water and in water/alcohol mixtures to produce oligomers and monomers of interest, at mild temperatures (200–275 °C) under inert atmosphere. It was found that the presence of alcohol and the type of alcohol (methanol, ethanol, isopropanol) greatly influenced the amount of oligomers and monomers formed from lignin, reaching a maximum of 48 mg·glignin−1 of monomers with isopropanol as a co-solvent. The impact of the addition of various solid catalysts composed of a metal phase (Pd, Pt or Ru) supported on an oxide (Al2O3, TiO2, ZrO2) was investigated. In water, the yield in monomers was enhanced by the presence of a catalyst and particularly by Pd/ZrO2. However, with an alcoholic co-solvent, the catalyst only enhanced the formation of oligomers. Detailed characterizations of the products with FTIR, 31P-NMR, 1H-NMR and HSQC NMR were performed to elucidate the chemical transformations occurring during solvolysis. The nature of the active catalytic specie was also investigated by testing homogeneous palladium catalysts. Full article
(This article belongs to the Special Issue Heterogeneous Catalysts for Lignin Upgrading)
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19 pages, 3762 KiB  
Article
Supported-Metal Catalysts in Upgrading Lignin to Aromatics by Oxidative Depolymerization
by Cédric Cabral Almada, Aleksandr Kazachenko, Pascal Fongarland, Denilson Da Silva Perez, Boris N. Kuznetsov and Laurent Djakovitch
Catalysts 2021, 11(4), 467; https://doi.org/10.3390/catal11040467 - 02 Apr 2021
Cited by 26 | Viewed by 3078
Abstract
Supported gold and platinum particles on titanium oxide catalysts were evaluated in the oxidative depolymerization of lignins toward high added value aromatics under mild conditions (T: 150 °C, Pair: 20 bar, CNaOH: 10 g/L, 1 h). Kraft and ethanol [...] Read more.
Supported gold and platinum particles on titanium oxide catalysts were evaluated in the oxidative depolymerization of lignins toward high added value aromatics under mild conditions (T: 150 °C, Pair: 20 bar, CNaOH: 10 g/L, 1 h). Kraft and ethanol Organosolv lignins were engaged in the study. Gold catalyst showed a strong tendency to further oxidize aromatics produced from lignin depolymerization to volatile compounds leading to very low yield in target molecules. On the contrary, platinum-based catalysts were allowed to observe enhanced yields that were attributed to its ability to preserve lignin’s substructure during the reaction. A kinetic model was constructed based on the results observed, which allowed us to identify the occurrence of condensation reactions during lignin oxidation and degradation of the produced aromatic compounds as the main limitations to reach high product yields. Insights on lignin oxidation and the catalyst’s role lead through this study would help to reach higher control over lignin valorization. Full article
(This article belongs to the Special Issue Heterogeneous Catalysts for Lignin Upgrading)
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