Tuning the Properties of Biobased PU Coatings via Selective Lignin Fractionation and Partial Depolymerization
Polyurethane (PU) coatings with high lignin content and tunable properties were made using a combination of fractionation and partial catalytic depolymerization as a novel strategy to tailor lignin molar mass and hydroxyl group reactivity, the key parameters for use in PU coatings. Acetone organosol...
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| Published in | ACS sustainable chemistry & engineering Vol. 11; no. 18; pp. 7193 - 7202 |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
08.05.2023
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Polyurethane (PU) coatings with high lignin content and tunable properties were made using a combination of fractionation and partial catalytic depolymerization as a novel strategy to tailor lignin molar mass and hydroxyl group reactivity, the key parameters for use in PU coatings. Acetone organosolv lignin obtained from pilot-scale fractionation of beech wood chips was processed at the kilogram scale to produce lignin fractions with specific molar mass ranges (M w 1000–6000 g/mol) and reduced polydispersity. Aliphatic hydroxyl groups were distributed relatively evenly over the lignin fractions, allowing detailed study of the correlation between lignin molar mass and hydroxyl group reactivity using an aliphatic polyisocyanate linker. As expected, the high molar mass fractions exhibited low cross-linking reactivity, yielding rigid coatings with a high glass transition temperature (T g). The lower M w fractions showed increased lignin reactivity, extent of cross-linking, and gave coatings with enhanced flexibility and lower T g. Lignin properties could be further tailored by lignin partial depolymerization by reduction (PDR) of the beech wood lignin and its high molar mass fractions; excellent translation of the PDR process was observed from laboratory to the pilot scale necessary for coating applications in prospective industrial scenarios. Lignin depolymerization significantly improved lignin reactivity, and coatings produced from PDR lignin showed the lowest T g values and highest coating flexibility. Overall, this study provides a powerful strategy for the production of PU coatings with tailored properties and high (>90%) biomass content, paving the path to the development of fully green and circular PU materials. |
|---|---|
| AbstractList | Polyurethane (PU)
coatings with high lignin content and tunable
properties were made using a combination of fractionation and partial
catalytic depolymerization as a novel strategy to tailor lignin molar
mass and hydroxyl group reactivity, the key parameters for use in
PU coatings. Acetone organosolv lignin obtained from pilot-scale fractionation
of beech wood chips was processed at the kilogram scale to produce
lignin fractions with specific molar mass ranges (
M
w
1000–6000 g/mol) and reduced polydispersity.
Aliphatic hydroxyl groups were distributed relatively evenly over
the lignin fractions, allowing detailed study of the correlation between
lignin molar mass and hydroxyl group reactivity using an aliphatic
polyisocyanate linker. As expected, the high molar mass fractions
exhibited low cross-linking reactivity, yielding rigid coatings with
a high glass transition temperature (
T
g
). The lower
M
w
fractions showed increased
lignin reactivity, extent of cross-linking, and gave coatings with
enhanced flexibility and lower
T
g
. Lignin
properties could be further tailored by lignin partial depolymerization
by reduction (PDR) of the beech wood lignin and its high molar mass
fractions; excellent translation of the PDR process was observed from
laboratory to the pilot scale necessary for coating applications in
prospective industrial scenarios. Lignin depolymerization significantly
improved lignin reactivity, and coatings produced from PDR lignin
showed the lowest
T
g
values and highest
coating flexibility. Overall, this study provides a powerful strategy
for the production of PU coatings with tailored properties and high
(>90%) biomass content, paving the path to the development of fully
green and circular PU materials.
Lignin
fractionation and partial depolymerization provide
a powerful strategy for the production of biobased PU coatings with
tailored properties. Polyurethane (PU) coatings with high lignin content and tunable properties were made using a combination of fractionation and partial catalytic depolymerization as a novel strategy to tailor lignin molar mass and hydroxyl group reactivity, the key parameters for use in PU coatings. Acetone organosolv lignin obtained from pilot-scale fractionation of beech wood chips was processed at the kilogram scale to produce lignin fractions with specific molar mass ranges ( 1000-6000 g/mol) and reduced polydispersity. Aliphatic hydroxyl groups were distributed relatively evenly over the lignin fractions, allowing detailed study of the correlation between lignin molar mass and hydroxyl group reactivity using an aliphatic polyisocyanate linker. As expected, the high molar mass fractions exhibited low cross-linking reactivity, yielding rigid coatings with a high glass transition temperature ( ). The lower fractions showed increased lignin reactivity, extent of cross-linking, and gave coatings with enhanced flexibility and lower . Lignin properties could be further tailored by lignin partial depolymerization by reduction (PDR) of the beech wood lignin and its high molar mass fractions; excellent translation of the PDR process was observed from laboratory to the pilot scale necessary for coating applications in prospective industrial scenarios. Lignin depolymerization significantly improved lignin reactivity, and coatings produced from PDR lignin showed the lowest values and highest coating flexibility. Overall, this study provides a powerful strategy for the production of PU coatings with tailored properties and high (>90%) biomass content, paving the path to the development of fully green and circular PU materials. Polyurethane (PU) coatings with high lignin content and tunable properties were made using a combination of fractionation and partial catalytic depolymerization as a novel strategy to tailor lignin molar mass and hydroxyl group reactivity, the key parameters for use in PU coatings. Acetone organosolv lignin obtained from pilot-scale fractionation of beech wood chips was processed at the kilogram scale to produce lignin fractions with specific molar mass ranges (Mw 1000-6000 g/mol) and reduced polydispersity. Aliphatic hydroxyl groups were distributed relatively evenly over the lignin fractions, allowing detailed study of the correlation between lignin molar mass and hydroxyl group reactivity using an aliphatic polyisocyanate linker. As expected, the high molar mass fractions exhibited low cross-linking reactivity, yielding rigid coatings with a high glass transition temperature (Tg). The lower Mw fractions showed increased lignin reactivity, extent of cross-linking, and gave coatings with enhanced flexibility and lower Tg. Lignin properties could be further tailored by lignin partial depolymerization by reduction (PDR) of the beech wood lignin and its high molar mass fractions; excellent translation of the PDR process was observed from laboratory to the pilot scale necessary for coating applications in prospective industrial scenarios. Lignin depolymerization significantly improved lignin reactivity, and coatings produced from PDR lignin showed the lowest Tg values and highest coating flexibility. Overall, this study provides a powerful strategy for the production of PU coatings with tailored properties and high (>90%) biomass content, paving the path to the development of fully green and circular PU materials.Polyurethane (PU) coatings with high lignin content and tunable properties were made using a combination of fractionation and partial catalytic depolymerization as a novel strategy to tailor lignin molar mass and hydroxyl group reactivity, the key parameters for use in PU coatings. Acetone organosolv lignin obtained from pilot-scale fractionation of beech wood chips was processed at the kilogram scale to produce lignin fractions with specific molar mass ranges (Mw 1000-6000 g/mol) and reduced polydispersity. Aliphatic hydroxyl groups were distributed relatively evenly over the lignin fractions, allowing detailed study of the correlation between lignin molar mass and hydroxyl group reactivity using an aliphatic polyisocyanate linker. As expected, the high molar mass fractions exhibited low cross-linking reactivity, yielding rigid coatings with a high glass transition temperature (Tg). The lower Mw fractions showed increased lignin reactivity, extent of cross-linking, and gave coatings with enhanced flexibility and lower Tg. Lignin properties could be further tailored by lignin partial depolymerization by reduction (PDR) of the beech wood lignin and its high molar mass fractions; excellent translation of the PDR process was observed from laboratory to the pilot scale necessary for coating applications in prospective industrial scenarios. Lignin depolymerization significantly improved lignin reactivity, and coatings produced from PDR lignin showed the lowest Tg values and highest coating flexibility. Overall, this study provides a powerful strategy for the production of PU coatings with tailored properties and high (>90%) biomass content, paving the path to the development of fully green and circular PU materials. Polyurethane (PU) coatings with high lignin content and tunable properties were made using a combination of fractionation and partial catalytic depolymerization as a novel strategy to tailor lignin molar mass and hydroxyl group reactivity, the key parameters for use in PU coatings. Acetone organosolv lignin obtained from pilot-scale fractionation of beech wood chips was processed at the kilogram scale to produce lignin fractions with specific molar mass ranges (M w 1000–6000 g/mol) and reduced polydispersity. Aliphatic hydroxyl groups were distributed relatively evenly over the lignin fractions, allowing detailed study of the correlation between lignin molar mass and hydroxyl group reactivity using an aliphatic polyisocyanate linker. As expected, the high molar mass fractions exhibited low cross-linking reactivity, yielding rigid coatings with a high glass transition temperature (T g). The lower M w fractions showed increased lignin reactivity, extent of cross-linking, and gave coatings with enhanced flexibility and lower T g. Lignin properties could be further tailored by lignin partial depolymerization by reduction (PDR) of the beech wood lignin and its high molar mass fractions; excellent translation of the PDR process was observed from laboratory to the pilot scale necessary for coating applications in prospective industrial scenarios. Lignin depolymerization significantly improved lignin reactivity, and coatings produced from PDR lignin showed the lowest T g values and highest coating flexibility. Overall, this study provides a powerful strategy for the production of PU coatings with tailored properties and high (>90%) biomass content, paving the path to the development of fully green and circular PU materials. |
| Author | Griffini, Gianmarco Smit, Arjan T. Dezaire, Thomas Hoek, Michiel Riddell, Luke A. Bellinetto, Emanuela Boumezgane, Oussama Turri, Stefano Bruijnincx, Pieter C. A. |
| AuthorAffiliation | Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry Department of Chemistry, Materials and Chemical Engineering “Giulio Natta” |
| AuthorAffiliation_xml | – name: Department of Chemistry, Materials and Chemical Engineering “Giulio Natta” – name: Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry |
| Author_xml | – sequence: 1 givenname: Arjan T. orcidid: 0000-0002-8685-3850 surname: Smit fullname: Smit, Arjan T. email: arjan.smit@tno.nl organization: Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry – sequence: 2 givenname: Emanuela surname: Bellinetto fullname: Bellinetto, Emanuela organization: Department of Chemistry, Materials and Chemical Engineering “Giulio Natta” – sequence: 3 givenname: Thomas surname: Dezaire fullname: Dezaire, Thomas organization: Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry – sequence: 4 givenname: Oussama surname: Boumezgane fullname: Boumezgane, Oussama organization: Department of Chemistry, Materials and Chemical Engineering “Giulio Natta” – sequence: 5 givenname: Luke A. surname: Riddell fullname: Riddell, Luke A. organization: Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry – sequence: 6 givenname: Stefano orcidid: 0000-0001-8996-0603 surname: Turri fullname: Turri, Stefano organization: Department of Chemistry, Materials and Chemical Engineering “Giulio Natta” – sequence: 7 givenname: Michiel surname: Hoek fullname: Hoek, Michiel – sequence: 8 givenname: Pieter C. A. orcidid: 0000-0001-8134-0530 surname: Bruijnincx fullname: Bruijnincx, Pieter C. A. organization: Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry – sequence: 9 givenname: Gianmarco orcidid: 0000-0002-9924-1722 surname: Griffini fullname: Griffini, Gianmarco email: gianmarco.griffini@polimi.it organization: Department of Chemistry, Materials and Chemical Engineering “Giulio Natta” |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/37180028$$D View this record in MEDLINE/PubMed |
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| CitedBy_id | crossref_primary_10_1002_slct_202301633 crossref_primary_10_1021_acssuschemeng_3c00619 crossref_primary_10_1021_acssuschemeng_3c00617 crossref_primary_10_1021_acssuschemeng_4c00303 crossref_primary_10_1039_D4SU00010B crossref_primary_10_1021_acssuschemeng_4c03100 crossref_primary_10_3390_polym16070947 |
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| Keywords | tunable PU coating properties biomass organosolv pretreatment lignin fractionation tailored lignin molar mass and reactivity reductive depolymerization |
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| Snippet | Polyurethane (PU) coatings with high lignin content and tunable properties were made using a combination of fractionation and partial catalytic... Polyurethane (PU) coatings with high lignin content and tunable properties were made using a combination of fractionation and partial catalytic... |
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| Title | Tuning the Properties of Biobased PU Coatings via Selective Lignin Fractionation and Partial Depolymerization |
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