{"title":"Silylated Softwood and Hardwood Lignin: Impact on Thermomechanical and Interfacial Properties of PLA Biocomposites.","authors":"Giulia Herbst, Gabriela Adriana Bastida, Quim Tarrés, Marcos Lúcio Corazza, Luiz Pereira Ramos, Marc Delgado-Aguilar","doi":"10.1021/acs.biomac.5c01179","DOIUrl":null,"url":null,"abstract":"<p><p>Achieving compatibility between biopolymers and natural fillers is a significant challenge in developing sustainable materials. PLA-lignin biocomposites frequently demonstrate poor interfacial adhesion, mostly due to polarity differences. Softwood (LS) and hardwood (LH) lignins vary in composition and reactivity, affecting PLA structure. This study evaluated the surface compatibilization of LS and LH through silylation at 1, 3, and 5 wt % using a GPS coupling agent. Silylation was validated by TGA, DSC (<i>T</i><sub>g</sub> increase of ∼3-7 °C), ash color, and EDX (increased silicon). FTIR assessed structural differences in lignins. Rheological tests and melt flow index indicated that unmodified lignin reduced PLA viscosity, while GPS-modified lignin increased it. DSC showed that LS enhanced crystallization more than LH, and GPS at 1 wt % promoted nucleation. Films containing LH at 10 and 1 wt % GPS exhibited improved mechanical properties. Barrier properties remained unchanged, though all films provided UV-blocking capability.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.4000,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Biomacromolecules","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.biomac.5c01179","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"BIOCHEMISTRY & MOLECULAR BIOLOGY","Score":null,"Total":0}
引用次数: 0
Abstract
Achieving compatibility between biopolymers and natural fillers is a significant challenge in developing sustainable materials. PLA-lignin biocomposites frequently demonstrate poor interfacial adhesion, mostly due to polarity differences. Softwood (LS) and hardwood (LH) lignins vary in composition and reactivity, affecting PLA structure. This study evaluated the surface compatibilization of LS and LH through silylation at 1, 3, and 5 wt % using a GPS coupling agent. Silylation was validated by TGA, DSC (Tg increase of ∼3-7 °C), ash color, and EDX (increased silicon). FTIR assessed structural differences in lignins. Rheological tests and melt flow index indicated that unmodified lignin reduced PLA viscosity, while GPS-modified lignin increased it. DSC showed that LS enhanced crystallization more than LH, and GPS at 1 wt % promoted nucleation. Films containing LH at 10 and 1 wt % GPS exhibited improved mechanical properties. Barrier properties remained unchanged, though all films provided UV-blocking capability.
期刊介绍:
Biomacromolecules is a leading forum for the dissemination of cutting-edge research at the interface of polymer science and biology. Submissions to Biomacromolecules should contain strong elements of innovation in terms of macromolecular design, synthesis and characterization, or in the application of polymer materials to biology and medicine.
Topics covered by Biomacromolecules include, but are not exclusively limited to: sustainable polymers, polymers based on natural and renewable resources, degradable polymers, polymer conjugates, polymeric drugs, polymers in biocatalysis, biomacromolecular assembly, biomimetic polymers, polymer-biomineral hybrids, biomimetic-polymer processing, polymer recycling, bioactive polymer surfaces, original polymer design for biomedical applications such as immunotherapy, drug delivery, gene delivery, antimicrobial applications, diagnostic imaging and biosensing, polymers in tissue engineering and regenerative medicine, polymeric scaffolds and hydrogels for cell culture and delivery.