Laccase-Catalyzed Copolymerization of Tannin and Technical Lignin: Polymerization Kinetics and Enhanced Properties of Polyphenols

Zonghong Lu, Jenni Tienaho, Petri Kilpeläinen, Luyao Wang, Hao Zhang, Liqiu Hu, Rui Liu, Hanna Brännström, Eelis Halmemies, Xiaoju Wang, Martti Toivakka*, Chunlin Xu*

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

8 Citations (Scopus)
21 Downloads (Pure)

Abstract

Polymerization of lignin has garnered significant interest due to its potential to unlock innovative and value-added applications for lignin to replace petroleum-based phenolic synthetics in future polymeric materials. However, conventional strategies for lignin polymerization often adopt complex cross-linking reactions with large amounts of unsustainable chemicals, which may impose environmental and ecological concerns. Herein, a green method for polyphenol polymerization is developed, in which tannin-rich extracts serve as building blocks to facilitate lignin polymerization under laccase-catalyzed oxidation. The molar mass and chemical structure of polymerized lignin, tannin, and their mixture and polymerization kinetics are comprehensively studied. Results show that the incorporation of tannin can increase the polymerization degree and rate of lignin and preserve more phenolic–OH groups after laccase incubation compared with self-polymerized lignin or tannin. Moreover, the possible polymerization mechanisms for lignin and tannin samples are proposed based on NMR and FTIR spectrum analysis. The polymerized lignin–tannin samples have superior or similar physicochemical properties compared to self-polymerized lignin or tannin in terms of UV shielding, thermal stability, and antimicrobial properties. Overall, this study offers novel insights into the copolymerization of lignin and tannin catalyzed by laccase and underpins further applications of upgraded polyphenols as polymers.
Original languageEnglish
Pages (from-to)8765-8779
Number of pages15
JournalACS Sustainable Chemistry and Engineering
Volume12
Issue number23
DOIs
Publication statusPublished - 29 May 2024
MoE publication typeA1 Journal article-refereed

Funding

Z.L. and L.H. would like to acknowledge the financial support from the China Scholarship Council (Student ID 202109370011 for Z.L. and Student ID 201908120107 for L.H.) to the doctoral study at \u00C5AU, Finland. C.X. would like to acknowledge the financial support provided by Business Finland (5855/31/2023) and by the European Union (Kesta\u0308va\u0308sti lisa\u0308a\u0308va\u0308a\u0308! - Turun lisa\u0308a\u0308va\u0308n valmistuksen osaamisen innovaatiokeskittyma\u0308) through European regional development fund (ERDF). The Research Council of Finland (ealier as Academy of Finland) funded project ForestAntivirals (342250) is acknowledge for providing resources for antibacterial testing. Ulla Jauhiainen (Luke, Finland) is acknowledged for proficient technical laboratory work with the antimicrobial analyses. CH-Bioforce Oy (Espoo, Finland) is thanked for providing birch alkaline lignin. Petri Ihalainen and Liji Sobhana Seleenmary Sobhanadhas (MetGen Oy, Finland) are acknowledged for providing the enzyme used in this study. This study is also part of the activities of the \u00C5bo Akademi University Foundation (S\u00C5A) funded Center of Excellence in Research \u201CMaterials-driven solutions for combating antimicrobial resistance (MADNESS)\u2033 at \u00C5AU. Parts of the research used Research Council of Finland Research Infrastructure \u201CPrinted Intelligence Infrastructure\u201D (PII-FIRI)

Keywords

  • lignin–tannin copolymerization
  • polyphenols
  • alkaliphilic laccase
  • antimicrobial polymer

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