Conversion of beechwood organosolv lignin via fast pyrolysis and in situ catalytic upgrading towards aromatic and phenolic-rich bio-oil
Lignin, an abundant renewable biopolymer found in plant cell walls, is enriched in phenolic units within its complex molecular structure. Unlocking its potential as alternative feedstock in (bio)refining has posed a long-standing challenge, even though it holds immense promise for replacing fossil-d...
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| Published in | Sustainable Chemistry for the Environment Vol. 6; p. 100107 |
|---|---|
| Main Authors | , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Elsevier B.V
01.06.2024
Elsevier |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Lignin, an abundant renewable biopolymer found in plant cell walls, is enriched in phenolic units within its complex molecular structure. Unlocking its potential as alternative feedstock in (bio)refining has posed a long-standing challenge, even though it holds immense promise for replacing fossil-derived phenolic and aromatic compounds. This study focuses on fast pyrolysis as effective thermochemical depolymerization method of lignin, coupled with the in situ catalytic upgrading aiming to produce valuable bio-oil enriched in dealkoxylated (alkyl)phenolic and aromatic compounds. Lignin was isolated via the organosolv process from beechwood sawdust (hardwood biomass). Various acidic aluminosilicate catalysts (e.g., zeolites, such as ZSM-5, Beta and USY, and amorphous silica alumina) were applied, having different Si/Al ratio, porous and acidic properties. Fast pyrolysis experiments were conducted on a fixed-bed bench-scale reactor at two distinct temperatures (500 and 600 °C), employing different contact times and lignin-to-catalyst ratios. Non-catalytic pyrolysis experiments revealed that higher temperature, significantly influences bio-oil’s composition and yield, resulting in the conversion of initially formed alkoxy-phenols to alkyl-phenolic compounds, reaching a 47% relative concentration at 600 °C, while also yielding high amount of bio-oil up to 43 wt%. Among the catalysts tested, zeolite ZSM-5 (Si/Al=40) proved to be the most efficient, shifting the chemical profile of bio-oil from phenolic to aromatic (mainly BTX) with relative concentration of 57%, owing to its unique microporous structure and acidity. Depending on the catalyst type, a balance between BTX monomer aromatics and naphthalenes was observed. Lignin, as well as the obtained products (bio-oil, non-condensable gases, char/coke-on-catalyst) were thoroughly characterized using various analytical techniques. The catalytic upgrading results were associated with the physicochemical properties of the catalysts, providing valuable insights into the underlying reaction mechanisms.
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| AbstractList | Lignin, an abundant renewable biopolymer found in plant cell walls, is enriched in phenolic units within its complex molecular structure. Unlocking its potential as alternative feedstock in (bio)refining has posed a long-standing challenge, even though it holds immense promise for replacing fossil-derived phenolic and aromatic compounds. This study focuses on fast pyrolysis as effective thermochemical depolymerization method of lignin, coupled with the in situ catalytic upgrading aiming to produce valuable bio-oil enriched in dealkoxylated (alkyl)phenolic and aromatic compounds. Lignin was isolated via the organosolv process from beechwood sawdust (hardwood biomass). Various acidic aluminosilicate catalysts (e.g., zeolites, such as ZSM-5, Beta and USY, and amorphous silica alumina) were applied, having different Si/Al ratio, porous and acidic properties. Fast pyrolysis experiments were conducted on a fixed-bed bench-scale reactor at two distinct temperatures (500 and 600 °C), employing different contact times and lignin-to-catalyst ratios. Non-catalytic pyrolysis experiments revealed that higher temperature, significantly influences bio-oil’s composition and yield, resulting in the conversion of initially formed alkoxy-phenols to alkyl-phenolic compounds, reaching a 47% relative concentration at 600 °C, while also yielding high amount of bio-oil up to 43 wt%. Among the catalysts tested, zeolite ZSM-5 (Si/Al=40) proved to be the most efficient, shifting the chemical profile of bio-oil from phenolic to aromatic (mainly BTX) with relative concentration of 57%, owing to its unique microporous structure and acidity. Depending on the catalyst type, a balance between BTX monomer aromatics and naphthalenes was observed. Lignin, as well as the obtained products (bio-oil, non-condensable gases, char/coke-on-catalyst) were thoroughly characterized using various analytical techniques. The catalytic upgrading results were associated with the physicochemical properties of the catalysts, providing valuable insights into the underlying reaction mechanisms.
[Display omitted] Lignin, an abundant renewable biopolymer found in plant cell walls, is enriched in phenolic units within its complex molecular structure. Unlocking its potential as alternative feedstock in (bio)refining has posed a long-standing challenge, even though it holds immense promise for replacing fossil-derived phenolic and aromatic compounds. This study focuses on fast pyrolysis as effective thermochemical depolymerization method of lignin, coupled with the in situ catalytic upgrading aiming to produce valuable bio-oil enriched in dealkoxylated (alkyl)phenolic and aromatic compounds. Lignin was isolated via the organosolv process from beechwood sawdust (hardwood biomass). Various acidic aluminosilicate catalysts (e.g., zeolites, such as ZSM-5, Beta and USY, and amorphous silica alumina) were applied, having different Si/Al ratio, porous and acidic properties. Fast pyrolysis experiments were conducted on a fixed-bed bench-scale reactor at two distinct temperatures (500 and 600 °C), employing different contact times and lignin-to-catalyst ratios. Non-catalytic pyrolysis experiments revealed that higher temperature, significantly influences bio-oil’s composition and yield, resulting in the conversion of initially formed alkoxy-phenols to alkyl-phenolic compounds, reaching a 47% relative concentration at 600 °C, while also yielding high amount of bio-oil up to 43 wt%. Among the catalysts tested, zeolite ZSM-5 (Si/Al=40) proved to be the most efficient, shifting the chemical profile of bio-oil from phenolic to aromatic (mainly BTX) with relative concentration of 57%, owing to its unique microporous structure and acidity. Depending on the catalyst type, a balance between BTX monomer aromatics and naphthalenes was observed. Lignin, as well as the obtained products (bio-oil, non-condensable gases, char/coke-on-catalyst) were thoroughly characterized using various analytical techniques. The catalytic upgrading results were associated with the physicochemical properties of the catalysts, providing valuable insights into the underlying reaction mechanisms. |
| ArticleNumber | 100107 |
| Author | Triantafyllidis, Konstantinos Christakopoulos, Paul Rova, Ulrika Margellou, Antigoni Pappa, Christina Matsakas, Leonidas Soldatos, Petros Torofias, Stylianos |
| Author_xml | – sequence: 1 givenname: Petros surname: Soldatos fullname: Soldatos, Petros organization: Department of Chemistry, Aristotle University of Thessaloniki, Thessaloniki 54124, Greece – sequence: 2 givenname: Antigoni surname: Margellou fullname: Margellou, Antigoni email: amargel@chem.auth.gr organization: Department of Chemistry, Aristotle University of Thessaloniki, Thessaloniki 54124, Greece – sequence: 3 givenname: Christina surname: Pappa fullname: Pappa, Christina organization: Department of Chemistry, Aristotle University of Thessaloniki, Thessaloniki 54124, Greece – sequence: 4 givenname: Stylianos surname: Torofias fullname: Torofias, Stylianos organization: Department of Chemistry, Aristotle University of Thessaloniki, Thessaloniki 54124, Greece – sequence: 5 givenname: Leonidas surname: Matsakas fullname: Matsakas, Leonidas organization: Biochemical Process Engineering, Division of Chemical Engineering, Department of Civil, Environmental and Natural Resources Engineering, Luleå University of Technology, Luleå 971-87, Sweden – sequence: 6 givenname: Ulrika surname: Rova fullname: Rova, Ulrika organization: Biochemical Process Engineering, Division of Chemical Engineering, Department of Civil, Environmental and Natural Resources Engineering, Luleå University of Technology, Luleå 971-87, Sweden – sequence: 7 givenname: Paul surname: Christakopoulos fullname: Christakopoulos, Paul organization: Biochemical Process Engineering, Division of Chemical Engineering, Department of Civil, Environmental and Natural Resources Engineering, Luleå University of Technology, Luleå 971-87, Sweden – sequence: 8 givenname: Konstantinos surname: Triantafyllidis fullname: Triantafyllidis, Konstantinos organization: Department of Chemistry, Aristotle University of Thessaloniki, Thessaloniki 54124, Greece |
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| CitedBy_id | crossref_primary_10_3390_catal15010048 crossref_primary_10_1016_j_biombioe_2025_107601 crossref_primary_10_1016_j_jaap_2024_106902 |
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| Keywords | In situ deoxygenation Hardwood lignin Microporous ZSM-5 Catalytic fast pyrolysis Organosolv lignin Phenols Bio-oil upgrading BTX aromatics |
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| SubjectTerms | Bio-oil upgrading Biochemical Process Engineering Biokemisk processteknik BTX aromatics Catalytic fast pyrolysis Hardwood lignin In situ deoxygenation Microporous ZSM-5 Organosolv lignin Phenols |
| Title | Conversion of beechwood organosolv lignin via fast pyrolysis and in situ catalytic upgrading towards aromatic and phenolic-rich bio-oil |
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