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<p>The transition toward environmentally responsible polymer production requires efficient strategies to transform renewable polyphenols into high-value biobased materials. However, enzymatic polymerization of tannins is often hindered by compositional variability in crude extracts, particularly by components that suppress laccase activity. This study demonstrates that solvent-assisted pretreatment is a decisive step for modulating the chemical composition of <i>Pinus radiata</i> bark tannins and, consequently, their enzymatic polymerization performance. Aqueous tannin extracts were subjected to controlled solvent-assisted pretreatment with solvents of increasing polarity, yielding fractions with distinct phenolic content and reactivity before polymerization. The pretreated fractions were characterized by FT-IR, TGA, Py-GC/MS, GC–MS, SEM, viscosity measurements, and water-solubility analyses to establish structure–reactivity relationships. Pretreatment conditions strongly influenced the relative abundance of phenolic and non-phenolic constituents, leading to pronounced differences in laccase-mediated polymer growth. Acetone-based pretreatment selectively preserved phenol-rich fractions, reaching viscosities of 1&#xa0;Pa·s after 40&#xa0;min of enzymatic reaction, while automated pretreatment enabled improved operational control and sequential fraction recovery. Short pretreatment times preserved phenolic integrity and enhanced polymerization efficiency, whereas prolonged pretreatment promoted partial oxidation and reduced enzymatic reactivity. Polymers obtained under optimized pretreatment conditions exhibited enhanced thermal stability, with a 20% increase in residual mass at 600&#xa0;°C, and reduced water solubility. Overall, these results confirm that targeted solvent-assisted pretreatment is a decisive strategy for efficient, scalable, and sustainable enzymatic polymerization of tannins.</p>

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Effect of Solvent-Assisted Pretreatment on the Laccase-Mediated Polymerization of Pinus radiata Bark Tannins

  • 期刊论文

  • 发表日期：

    2026年7月11日

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  • Myleidi Vera,
  • Carolina Guiñez,
  • Edison Monroy,
  • Lisette Lagos,
  • Rayen Holder,
  • Cristina Segura,
  • Romina Romero

摘要

The transition toward environmentally responsible polymer production requires efficient strategies to transform renewable polyphenols into high-value biobased materials. However, enzymatic polymerization of tannins is often hindered by compositional variability in crude extracts, particularly by components that suppress laccase activity. This study demonstrates that solvent-assisted pretreatment is a decisive step for modulating the chemical composition of Pinus radiata bark tannins and, consequently, their enzymatic polymerization performance. Aqueous tannin extracts were subjected to controlled solvent-assisted pretreatment with solvents of increasing polarity, yielding fractions with distinct phenolic content and reactivity before polymerization. The pretreated fractions were characterized by FT-IR, TGA, Py-GC/MS, GC–MS, SEM, viscosity measurements, and water-solubility analyses to establish structure–reactivity relationships. Pretreatment conditions strongly influenced the relative abundance of phenolic and non-phenolic constituents, leading to pronounced differences in laccase-mediated polymer growth. Acetone-based pretreatment selectively preserved phenol-rich fractions, reaching viscosities of 1 Pa·s after 40 min of enzymatic reaction, while automated pretreatment enabled improved operational control and sequential fraction recovery. Short pretreatment times preserved phenolic integrity and enhanced polymerization efficiency, whereas prolonged pretreatment promoted partial oxidation and reduced enzymatic reactivity. Polymers obtained under optimized pretreatment conditions exhibited enhanced thermal stability, with a 20% increase in residual mass at 600 °C, and reduced water solubility. Overall, these results confirm that targeted solvent-assisted pretreatment is a decisive strategy for efficient, scalable, and sustainable enzymatic polymerization of tannins.