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<p>Enzymatic phenolic polymerization provides a versatile route to functional aromatic polymers under mild conditions. However, it remains unclear whether polymer structure and properties are governed mainly by the enzyme species or by structural features of the phenolic monomers. This review reorganizes prior studies using a monomer-structure-guided framework, focusing on the number and accessibility of reactive positions on phenolic rings rather than on enzymes. Enzymes are highlighted primarily as oxidative activators, whereas polymer growth and cross-linking are predominantly determined by monomer structure. For monophenols, the availability of ortho and para positions controls architecture, and formation of highly cross-linked networks (gelation/insolubilization) is generally suppressed when both ortho positions are effectively blocked, as in 2,6-disubstituted phenols. In contrast, polyphenolic monomers such as catechol and hydroquinone are dominated by quinone formation and subsequent secondary reactions, indicating limitations of simple radical coupling descriptions. The review further links polymer architecture to functional outcomes including antioxidant activity, metal-binding capability, and bio-related functions, and discusses challenges and perspectives for material-oriented development. Key remaining challenges include robust structural characterization, molecular-weight evaluation, reproducibility, and solubility control, which are critical for reliable structure–property correlations and application-oriented development.</p>

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Enzymatic synthesis of phenolic polymers: structures, properties, and applications

  • 期刊论文

  • 发表日期：

    2026年5月11日

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  • Hiroyuki Tonami

摘要

Enzymatic phenolic polymerization provides a versatile route to functional aromatic polymers under mild conditions. However, it remains unclear whether polymer structure and properties are governed mainly by the enzyme species or by structural features of the phenolic monomers. This review reorganizes prior studies using a monomer-structure-guided framework, focusing on the number and accessibility of reactive positions on phenolic rings rather than on enzymes. Enzymes are highlighted primarily as oxidative activators, whereas polymer growth and cross-linking are predominantly determined by monomer structure. For monophenols, the availability of ortho and para positions controls architecture, and formation of highly cross-linked networks (gelation/insolubilization) is generally suppressed when both ortho positions are effectively blocked, as in 2,6-disubstituted phenols. In contrast, polyphenolic monomers such as catechol and hydroquinone are dominated by quinone formation and subsequent secondary reactions, indicating limitations of simple radical coupling descriptions. The review further links polymer architecture to functional outcomes including antioxidant activity, metal-binding capability, and bio-related functions, and discusses challenges and perspectives for material-oriented development. Key remaining challenges include robust structural characterization, molecular-weight evaluation, reproducibility, and solubility control, which are critical for reliable structure–property correlations and application-oriented development.