After cellulose, lignin is the most commonly used natural polymer in green biomaterials. Pulp and paper mills and emerging cellulosic biorefineries are the main sources of technical lignin. However, only 2–5% of lignin has been converted into biomaterials. Making lignin-based polymer biocomposites to replace petroleum-based composites has piqued the interest of many researchers worldwide due to the positive environmental impact of traditional composites over time. In composite development, lignin is being used as a filler in commercial polymers to improve biodegradability and possibly lower production costs. As a natural polymer, lignin may have different properties depending on the isolation method and source, affecting polymer-based composites. The application has been affected by the characteristics of lignin and the uniform distribution of lignin in polymers. The review’s goal was to provide an overview of technical lignin extraction, properties, and its potential appropriate utilization. It was also planned to revisit the lignin-based composites’ preparation procedure as well as their composite characteristics. Solvent casting and extrusion methods are used to fabricate lignin from polymeric matrices such as polypropylene, epoxy, polyvinyl alcohol, polylactic acid, starch, wood fiber, natural rubber, and chitosan. Packaging, biomedical materials, automotive, advanced biocomposites, flame retardant, and other applications for lignin-based composites has existed. As a result, the technology is still being refined to increase the performance of lignin-based biocomposites in several applications. This review could assist explain lignin’s position as a composite additive, which could lead to more efficient processing and application strategies.

Lignin has potential as a reinforcing filler and to become an alternative to carbon black in the rubber industry. This is because it is formed from cheaper materials with abundant annually renewable sources and has low weight, high biological efficiency, and wide ecological adaptability. The utilization of bio-filler in the rubber industry has garnered increasing attention from researchers due to increasing environmental concerns over the toxic effects of carbon black on health and the environment. This article is intended to summarize current efforts in the development of a green and sustainable rubber product. Instead of focusing on silica and alternative rubber matrix-like guayule and Russian dandelion, it looks at lignin, which also has potential as a reinforcing filler and can enable the development of competitive green rubber composites. Lignin has several special characteristics such as good mechanical, physico-chemical, biodegradability, and antioxidant properties and excellent thermal stability. However, the incorporation of lignin in a rubber matrix is not straightforward, and this needs to be overcome with certain suitable solutions because of the polarity of lignin molecules, which contributes to strong self-interactions. Consequently, chemical modification of lignin is often used to improve the dispersion of lignin in elastomers, or a compatibilizer is added to enhance interfacial adhesion between lignin and the rubber matrix. This review attempts to compile relevant knowledge about the performance of lignin-filled rubber composite using different approaches such as mixing method, surface modification, hybrid fillers, etc. This study is expected to gain significant interest from researchers globally on the subject of lignin-based rubber composites and the advancement of development in green rubber products.

Kraft lignin was modified by using hydroxymethylation to enhance the compatibility between rubber based on a blend of natural rubber/polybutadiene rubber (NR/BR) and lignin. To confirm this modification, the resultant hydroxymethylated kraft lignin (HMKL) was characterized using Fourier transform infrared (FTIR) and nuclear magnetic resonance (NMR) spectroscopy. It was then incorporated into rubber composites and compared with unmodified rubber. All rubber composites were investigated in terms of rheology, mechanical properties, aging, thermal properties, and morphology. The results show that the HMKL influenced the mechanical properties (tensile properties, hardness, and compression set) of NR/BR composites compared to unmodified lignin. Further evidence also revealed better dispersion and good interaction between the HMKL and the rubber matrix. Based on its performance in NR/BR composites, hydroxymethylated lignin can be used as a filler in the rubber industry.

Halloysite nanotubes (HNTs) are naturally occurring tubular clay made of aluminosilicate sheets rolled several times. HNT has been used to reinforce many rubbers. However, the narrow diameter of this configuration causes HNT to have poor interfacial contact with the rubber matrix. Therefore, increasing the distance between layers could improve interfacial contact with the matrix. In this work, Epoxidized Natural Rubber (ENR)/HNT was the focus. The HNT layer distance was successfully increased by a urea-mechanochemical process. Attachment of urea onto HNT was verified by FTIR, where new peaks appeared around 3505 cm⁻¹ and 3396 cm⁻¹, corresponding to urea’s functionalities. The intercalation of urea to the distance gallery of HNT was revealed by XRD. It was also found that the use of urea-treated HNT improved the modulus, tensile strength, and tear strength of the composites. This was clearly responsible for interactions between ENR and urea-treated HNT. It was further verified by observing the Payne effect. The value of the Payne effect was found to be reduced at 62.38% after using urea for treatment. As for the strain-induced crystallization (SIC) of the composites, the stress–strain curves correlated well with the results from synchrotron wide-angle X-ray scattering.