JEONG, KIM MIN Lee, Young A. Wu, Jie Kim, Hyeyun Ko, Ja Kyong Moon, Myoung-Woon Yoo, Chang Geun Jeong, Keunhong Kim, Kwang Ho 2025-01-17T05:00:19Z 2025-01-17T05:00:19Z 2025-01-15 2025-01 https://pubs.kist.re.kr/handle/201004/151566 Fully renewable hydrophobic materials offer a promising solution to addressing environmental challenges. Lignin, a relatively underutilized renewable polymer that naturally exhibits hydrophobicity, shows potential as a blend material in various applications. However, current approaches using technical lignin as a primary component or additive in renewable film manufacturing often rely on nonrenewable, external hydrophobic agents. Here, we developed a tandem strategy to create a fully renewable, hydrophobic lignin-based film. First, lignin was esterified by incorporating long-chain palmitic groups to enhance its hydrophobicity. A poly[(R)-3-hydroxybutyrate] (PHB) film containing 20% palmitoylated lignin demonstrated improved hydrophobicity, with the water contact angle (WCA) increasing from 75.4 to 106.7°. To further enhance hydrophobicity, the film underwent oxygen plasma treatment, which introduced macroscopic surface roughness in the form of “nanoforests.” This treatment significantly increased the WCA to 139°, confirming the effectiveness of the tandem strategy for producing hydrophobic 2D materials. Molecular dynamics simulations revealed that the C16 chain in palmitoylated lignin created a more compact complex with PHB through strong van der Waals interactions and optimized hydrogen bonding, suggesting potential for developing high-lignin-content films. This work demonstrates a facile approach for fabricating fully renewable, hydrophobic composite films without the need for external materials. English AMER CHEMICAL SOC Fabrication of Hydrophobic Lignin-Based Films through Tandem Chemical Modification and Plasma Treatment Article 10.1021/acsapm.4c03574 1 ACS Applied Polymer Materials, v.7, no.1, pp.503 - 511 ACS Applied Polymer Materials 7 1 503 511 N scie scopus 001383197200001 Materials Science, Multidisciplinary Polymer Science Materials Science Polymer Science Article WATER PERFORMANCE NANOFIBRILS IMPROVEMENT COMPOSITES SURFACES BARRIER FILLER hydrophobicity plasma etching palmitoylation lignin valorization lignin