Tuning the Properties of Biobased PU Coatings via Selective Lignin Fractionation and Partial Depolymerization

Arjan T. Smit*, Emanuela Bellinetto, Thomas Dezaire, Oussama Boumezgane, Luke A. Riddell, Stefano Turri, Michiel Hoek, Pieter C.A. Bruijnincx, Gianmarco Griffini*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

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 (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.

Original languageEnglish
Pages (from-to)7193-7202
Number of pages10
JournalACS Sustainable Chemistry and Engineering
Volume11
Issue number18
DOIs
Publication statusPublished - 8 May 2023

Bibliographical note

Funding Information:
This project has received funding provided by the Netherlands Ministry of Economic Affairs as part of TNO’s biomass research program, by Regione Lombardia and Fondazione Cariplo (Grant Number 2018-1739, Project: POLISTE), and by the European Union’s Horizon 2020 Research and Innovation Programme (Grant Agreement No. 952941, Project: BIOMAC). The authors are grateful to the following persons for their excellent contribution to this work: Petra Bonouvrie, Ron van der Laan, Karina Vogelpoel-de Wit, Ben van Egmond, Dr. Kerstin Thiele, and Dr. André van Zomeren.

Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.

Funding

This project has received funding provided by the Netherlands Ministry of Economic Affairs as part of TNO’s biomass research program, by Regione Lombardia and Fondazione Cariplo (Grant Number 2018-1739, Project: POLISTE), and by the European Union’s Horizon 2020 Research and Innovation Programme (Grant Agreement No. 952941, Project: BIOMAC). The authors are grateful to the following persons for their excellent contribution to this work: Petra Bonouvrie, Ron van der Laan, Karina Vogelpoel-de Wit, Ben van Egmond, Dr. Kerstin Thiele, and Dr. André van Zomeren.

FundersFunder number
Netherlands Ministry of Economic Affairs as part of TNO's biomass research program
Regione Lombardia
Fondazione Cariplo2018-1739
European Union952941

    Keywords

    • biomass organosolv pretreatment
    • lignin fractionation
    • reductive depolymerization
    • tailored lignin molar mass and reactivity
    • tunable PU coating properties

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