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Polymers
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Advanced Study on Lignin-Containing Composites
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Advanced Study on Lignin-Containing Composites

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Biobased and Biodegradable Polymers".

Deadline for manuscript submissions: 15 June 2026 | Viewed by 6793

Special Issue Editors

Dr. Florian Zikeli

E-Mail Website
Guest Editor
Department of Civil and Environmental Engineering, University of Perugia, 05100 Terni, Italy
Interests: lignin; wood chemistry; lignocellulose; lignin nanoparticles; biocomposites; bio-based polymers
Special Issues, Collections and Topics in MDPI journals
Dr. Debora Puglia

E-Mail Website1 Website2
Guest Editor
Department of Civil and Environmental Engineering, University of Perugia, 05100 Terni, Italy
Interests: bionanocomposites; natural fibers composites; lignin nanoparticles; nanocellulose; active packaging; polymeric nanocomposites
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Aromatic lignin, along with structural polysaccharides such as cellulose and hemicellulose, contribute to the exceptional strength of plant cell walls on the nanoscale and wood on the macroscopic scale, providing humanity with a versatile building and crafting material for thousands of years.

The extensive processing of lignocellulosic biomass for various uses, including construction, pulp and paper, and food production, results in significant residual biomass and, in particular, lots of lignin in side and waste streams. This byproduct has recently been increasingly utilized as a foundational element for developing specialized materials tailored to address specific research applications.

The purpose of this Special Issue is to explore a wide range of lignin-based or lignin-containing polymer composites that have been applied to tackle contemporary, innovative research challenges within the context of a circular bioeconomy. Original research and review articles are welcome.

Dr. Florian Zikeli
Dr. Debora Puglia
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 250 words) can be sent to the Editorial Office for assessment.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • lignin
  • biobased polymers
  • biocomposites
  • lignocellulose
  • cross-linked polymers
  • phenolic compounds
  • resins

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Published Papers (6 papers)

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Research

25 pages, 4445 KB  
Article
Sustainable Protective Composite Textiles: Valorizing Hemp Hurd and Corn Stover Lignin via Electrospinning
by Dorota B. Szlek, Nara Han, Chang Geun Yoo and Margaret W. Frey
Polymers 2026, 18(9), 1124; https://doi.org/10.3390/polym18091124 - 2 May 2026
Viewed by 972
Abstract
Valorization of abundant agricultural residues, particularly lignin, provides the opportunity to divert waste streams while enabling materials to inherently exhibit durable functionalities, including UV-blocking, antioxidant properties and water repellency. This study reports the side-by-side valorization of hemp hurd (HL) and corn stover lignin [...] Read more.
Valorization of abundant agricultural residues, particularly lignin, provides the opportunity to divert waste streams while enabling materials to inherently exhibit durable functionalities, including UV-blocking, antioxidant properties and water repellency. This study reports the side-by-side valorization of hemp hurd (HL) and corn stover lignin (CL), extracted using the CELF process, into electrospun lignin/nylon 6 nanofiber membranes, establishing how lignin botanical origin, molecular weight (Mw), and blend ratio govern multifunctional performance relevant to protective membranes in textiles. Lignin–nylon 6 hydrogen bonding was regulated by the OH content and accessibility, Mw, and purity, and influenced the functional properties of the fibers. While stronger in low-Mw nanofibers, these interactions were weakest in low-Mw HL samples due to the lowest purity, despite the highest OH content. Fibers with low-Mw lignin yielded finer, brittle fibers with higher UV blocking, whereas high-Mw fractions showed higher antioxidant performance due to decreased interactions with nylon 6. Overall, lignin/nylon 6 nanofiber membranes delivered biobased UPF 50+ performance, 55–61% antioxidant activity at the optimal concentration, and exhibited tunable water repellency via fraction selection and the blend ratio. In combination with a nanofiber architecture, these membranes can impart durable inherent functionality onto textile substrates without affecting their existing properties, including water vapor permeability, without the use of chemical finishing, while utilizing renewable resources from agricultural residues. Full article
(This article belongs to the Special Issue Advanced Study on Lignin-Containing Composites)
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20 pages, 6526 KB  
Article
Synthesis and Application of Kraft Lignin-Based Polyurethane Coatings for Functional Paper Packaging Materials
by Julia de Cristo Figueiredo, Fernando José Borges Gomes, Ericka Figueiredo Alves Redmond, Biljana Bujanovic, Roberto Carlos Costa Lelis, Mayara Felix Santana and Clayton Mickles
Polymers 2026, 18(7), 787; https://doi.org/10.3390/polym18070787 - 25 Mar 2026
Viewed by 580
Abstract
The packaging sector presents a significant sustainability challenge, particularly due to the prevalence of plastic packaging. There is a growing interest in sustainable packaging alternatives. The main challenge is to develop packaging with comparable and competitive characteristics. In this context, this manuscript aims [...] Read more.
The packaging sector presents a significant sustainability challenge, particularly due to the prevalence of plastic packaging. There is a growing interest in sustainable packaging alternatives. The main challenge is to develop packaging with comparable and competitive characteristics. In this context, this manuscript aims to evaluate the performance of lignin-based polyurethane applied as a coating on recycled linerboard. Industrial softwood kraft lignin was fully characterized in terms of purity, functional groups (FTIR and 31P NMR) and molecular weight (GPC). Aiming at coating applications, the lignin sample was solubilized in dimethyl sulfoxide (DMSO) and used as a polyol substitute in the reaction, replacing polyethylene glycol (PEG) at levels of 70%, 80%, and 90%. Subsequently, hexamethylene diisocyanate (HDI) was added to initiate polyurethane formation. After polymerization, the coating was applied in multiple layers onto the linerboard paper. Regarding water resistance, all applications demonstrated effectiveness. The lignin-based polyurethane coating improved the Cobb1800 with reductions in the range of 1147.4 to 1155.8 g/m2 compared to the uncoated paper. Water vapor permeability was reduced by more than 94%. In the evaluation of oil resistance, samples with three layers and 90% lignin replacement performed particularly well, achieving a high value in a kit test for oil and grease (kit test number 12). These results highlight a promising approach to paper-based packaging, with potential applications across a wide range of products. Full article
(This article belongs to the Special Issue Advanced Study on Lignin-Containing Composites)
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12 pages, 2320 KB  
Article
Multifunctional Performance Lignin-Crosslinked-PVA Composite Film Based on a Dual Crosslinking Network
by Weipeng Yao, Shuzhen Ni, Yongchao Zhang and Yingjuan Fu
Polymers 2026, 18(5), 605; https://doi.org/10.3390/polym18050605 - 28 Feb 2026
Viewed by 652
Abstract
The development of high-performance biocomposites based on poly vinyl alcohol (PVA) and lignin is often hindered by the limited interfacial compatibility. Herein, we reporte a synchronized crosslinking strategy to seamlessly integrate lignin and PVA into a uniform and robust composite film. The vinyl [...] Read more.
The development of high-performance biocomposites based on poly vinyl alcohol (PVA) and lignin is often hindered by the limited interfacial compatibility. Herein, we reporte a synchronized crosslinking strategy to seamlessly integrate lignin and PVA into a uniform and robust composite film. The vinyl groups were introduced into both lignin and PVA molecular chains, which enable the formation of dense covalent bonds through reactions between these unsaturated carbon–carbon double bonds. This dual network structure combining covalent crosslinking with hydrogen bonding effectively strengthened the interfacial compatibility between lignin and PVA, which substantially enhanced film toughness, exhibiting an elongation at break of up to 4300%. Furthermore, the prepared composite film also demonstrated outstanding UV-blocking efficiency (>90%), strong antioxidant activity (82% DPPH scavenging), enhanced hydrophobicity (water contact angle of 97.9°), and improved thermal stability. The dramatic enhancements were attributed to the homogeneous dispersion of modified lignin within the covalently bonded network, which ensured efficient stress transfer and reduced the availability of hydrophilic groups. This synchronized crosslinking approach presents a versatile and effective route for fabricating high-value lignin-based composite materials. Full article
(This article belongs to the Special Issue Advanced Study on Lignin-Containing Composites)
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21 pages, 4659 KB  
Article
Effect of Different Aqueous Solvents with and Without Solubilized Lignin on the Swelling Behavior of Holocellulose Fibers
by Cornelia Hofbauer, Thomas Harter, Ulrich Hirn, Michael Harasek, Luis Zelaya-Lainez, Josef Füssl, Markus Lukacevic and Sebastian Serna-Loaiza
Polymers 2025, 17(23), 3103; https://doi.org/10.3390/polym17233103 - 22 Nov 2025
Cited by 1 | Viewed by 1195
Abstract
The modification of lignocellulosic fibers through controlled swelling and impregnation plays a decisive role in tailoring their structure and reactivity for use in sustainable composite materials. In this study, holocellulose fibers were swollen in various solvents (sodium hydroxide at 2 and 4 wt% [...] Read more.
The modification of lignocellulosic fibers through controlled swelling and impregnation plays a decisive role in tailoring their structure and reactivity for use in sustainable composite materials. In this study, holocellulose fibers were swollen in various solvents (sodium hydroxide at 2 and 4 wt% and ethanol–water mixtures at 0, 50, 70, and 100 wt%) to evaluate their impact on swelling and fiber characteristics. The pulp was produced with peracetic acid at 90 °C for 120 min from spruce wood chips and used for the swelling treatment. The fibers underwent swelling for 4 h in the different solvents, both without and with solubilized lignin at concentrations of 10 and 30 g/L, to investigate the impregnation ability of the fibers for lignin as a natural binder. Fiber morphology, lignocellulosic composition, and liquid retention values were analyzed to assess the effects of solvent–binder interactions on fiber swelling and lignin uptake. The results revealed significant differences in fiber characteristics influenced by both solvent choice and lignin presence, demonstrating the feasibility and optimization potential of a single-step swelling-impregnation process. These findings highlight key factors that can improve the uptake of natural binders in wood fibers, offering insights for effective fiber preconditioning in composite production. Full article
(This article belongs to the Special Issue Advanced Study on Lignin-Containing Composites)
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23 pages, 3230 KB  
Article
A Multi-Analytical Study of Nanolignin/Methylcellulose-Coated Groundwood and Cotton Linter Model Papers
by Mia Bloss, Marianne Odlyha and Charis Theodorakopoulos
Polymers 2025, 17(21), 2934; https://doi.org/10.3390/polym17212934 - 31 Oct 2025
Viewed by 1074
Abstract
This paper presents the synthesis of sustainable lignin nanoparticles (LNPs) and their application in methylcellulose (MC) as LNP/MC coatings for handmade papers. LNPs were produced from bulk kraft lignin via an acetone/water and sonication method, then incorporated into a 1 wt% methylcellulose (MC) [...] Read more.
This paper presents the synthesis of sustainable lignin nanoparticles (LNPs) and their application in methylcellulose (MC) as LNP/MC coatings for handmade papers. LNPs were produced from bulk kraft lignin via an acetone/water and sonication method, then incorporated into a 1 wt% methylcellulose (MC) matrix at concentrations of 0.4, 1, and 2 wt%. Groundwood and cotton linter papers were coated and exposed to 90 °C and 45% relative humidity (RH) for 16 days and the samples’ response to ageing at different concentrations of nanolignin was tested using a multi-analytical approach. The morphology of the LNPs was revealed with scanning electron microscopy, and most LNPs measured below a diameter of 30.8 nm. Colourimetry showed coated samples were inherently darker than uncoated samples but mostly stable in colour. pH remained near neutral for coated groundwood papers during ageing, but cotton papers were consistently acidic. Fourier transform infrared (FTIR) spectroscopy identified spectral similarities between uncoated and coated groundwood samples at approximately 1635 cm–1 and 1725 cm–1, attributed to carbonyl and carboxyl groups, suggesting that LNPs did not contribute to the formation of these groups during ageing. Controlled environment dynamic mechanical analysis (DMA-RH) found improved consolidation and lower elongation in most LNP/MC-treated samples. These results indicate that there may be potential for LNPs within paper conservation. Full article
(This article belongs to the Special Issue Advanced Study on Lignin-Containing Composites)
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17 pages, 15586 KB  
Article
Wheat Straw Lignin Nanoparticles as Active Filler in Thermoplastic Starch Films
by Florian Zikeli, Franco Dominici, Marco Rallini, Sebastian Serna-Loaiza, Walter Wukovits, Anton Friedl, Michael Harasek, Luigi Torre and Debora Puglia
Polymers 2025, 17(17), 2308; https://doi.org/10.3390/polym17172308 - 26 Aug 2025
Viewed by 1297
Abstract
Starch and lignin are promising biopolymers for the production of biodegradable biocomposite materials. The possibility of processing starch into thermoplastic materials qualifies it as a starting material for the preparation of thermoplastic packaging films, and the combination with lignin can even out some [...] Read more.
Starch and lignin are promising biopolymers for the production of biodegradable biocomposite materials. The possibility of processing starch into thermoplastic materials qualifies it as a starting material for the preparation of thermoplastic packaging films, and the combination with lignin can even out some inherent weak points of starch, such as moisture and water sensitivity, and can add additional features like antioxidant activity. Lignins from herbaceous biomass carry building blocks that are not found in wood lignins and are known for their bioactivity, such as p-coumaric acid or ferulic acid. In this work, a protocol was developed to initially prepare hybrids of wheat starch granules and lignin nanoparticles, which were then plasticized using glycerol in an extrusion process to produce thin films. The lignin-containing thermoplastic starch films showed higher Young’s moduli and less elongation at break compared to neat thermoplastic starch films, while tensile strength remained at the level of the neat films. Thermal stability was slightly increased by lignin addition, and oxygen transmission rates were low for lignin contents as low as 1 wt%. The hydrophobicity of the lignin-containing films increased strongly, and they showed an elevated antioxidant activity over several hours, which was also maintained after 24 h. The preparation of hybrid wheat starch lignin particles was successfully tested for the extrusion of thermoplastic starch films with improved thermomechanical properties, decreased water sensitivity, and prolonged antioxidant activity. Full article
(This article belongs to the Special Issue Advanced Study on Lignin-Containing Composites)
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