Latest Advancements in the Development of High-Performance Lignin- and Tannin-Based Non-Isocyanate Polyurethane Adhesive for Wood Composites.

The depletion of natural resources and increasing environmental apprehension regarding the reduction of harmful isocyanates employed in manufacturing polyurethanes (PUs) have generated significant attention from both industrial and academic sectors. This attention is focused on advancing bio-based non-isocyanate polyurethane (NIPU) resins as viable and sustainable substitutes, possessing satisfactory properties. This review presents a comprehensive analysis of the progress made in developing bio-based NIPU polymers for wood adhesive applications. The main aim of this paper is to conduct a comprehensive analysis of the latest advancements in the production of high-performance bio-based NIPU resins derived from lignin and tannin for wood composites. A comprehensive evaluation was conducted on scholarly publications retrieved from the Scopus database, encompassing the period from January 2010 to April 2023. In NIPU adhesive manufacturing, the exploration of substitute materials for isocyanates is imperative, due to their inherent toxicity, high cost, and limited availability. The process of demethylation and carbonation of lignin and tannin has the potential to produce polyphenolic compounds that possess hydroxyl and carbonyl functional groups. Bio-based NIPUs can be synthesized through the reaction involving diamine molecules. Previous studies have provided evidence indicating that NIPUs derived from lignin and tannin exhibit enhanced mechanical properties, decreased curing temperatures and shortened pressing durations, and are devoid of isocyanates. The characterization of NIPU adhesives based on lignin and tannin was conducted using various analytical techniques, including Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), matrix-assisted laser desorption/ionization with time-of-flight (MALDI-TOF) mass spectrometry, and gel permeation chromatography (GPC). The adhesive performance of tannin-based NIPU resins was shown to be superior to that of lignin-based NIPUs. This paper elucidates the potential of lignin and tannin as alternate sources for polyols in the manufacturing of NIPUs, specifically for their application as wood adhesives.

Synthesis of Jatropha-Oil-Based Polyester Polyol as Sustainable Biobased Material for Waterborne Polyurethane Dispersion.

The utilization of vegetable oil in the production of polymeric material has gained interest due to its proven ability to replace nonrenewable petroleum sources, as it is readily modified via chemical reaction to produce polyol and subsequently for polyurethane production. Jatropha oil (JO), a second-generation feedstock, is one of the suitable candidates for polyester polyol synthesis because it contains a high percentage of unsaturated fatty acids. In this study, jatropha-based polyester polyols (JOLs) with different hydroxyl values were successfully synthesized via a two-step method: epoxidation followed by oxirane ring-opening reaction. Ring-opening reagents; methanol, ethanol, and isopropanol were used to produce polyol with hydroxyl number of 166, 180, and 189 mg/KOH, respectively. All the synthesized JOLs exhibited a Newtonian to shear thinning behavior in the measured shear rate ranges from 10 to 1000 s-1 at 25 °C. The viscosity of a JOL ring-opened with methanol, isopropanol, and ethanol was 202, 213, and 666 mPa·s, respectively, at 20 °C and 100 s-1, which is within the range of commercially available polyols. Successively, the JOLs were reacted with isophorone diisocyanate (IPDI) to produce polyurethane prepolymer by utilizing 2,2-dimethylol propionic acid (DMPA) as an emulsifier. The prepolymer was then dispersed in water to produce a waterborne polyurethane dispersion. Colloidal stability of the jatropha-based polyurethane dispersions (JPUDs) were investigated by particle size analysis. A JPUD with a small particle size in the range of 6.39 to 43.83 nm was obtained, and the trend was associated with the soft segment of the polyol in the formulation. The zeta potentials of the JPUs ranged from -47.01 to -88.9 mV, indicating that all synthesized JPUs had high dispersity and stability. The efficient synthesis procedure, low cost, and excellent properties of the resulting product are thought to offer an opportunity to use jatropha oil as a sustainable resource for polyester polyol preparation.

Ternary Nanocomposite System Composing of Graphene Nanoplatelet, Cellulose Nanofiber and Jatropha Oil Based Waterborne Polyurethane: Characterizations, Mechanical, Thermal Properties and Conductivity.

This work aims to evaluate the performance of graphene nanoplatelet (GNP) as conductive filler with the presence of 0.5 wt.% cellulose nanofiber (CNF) on the physical, mechanical, conductivity and thermal properties of jatropha oil based waterborne polyurethane. Polyurethane was made from crude jatropha oil using an epoxidation and ring-opening process. 0.5, 1.0, 1.5, 2.0 wt.% GNP and 0.5 wt.% CNF were incorporated using casting method to enhance film performance. Mechanical properties were studied following standard method as stated in ASTM D638-03 Type V. Thermal stability of the nanocomposite system was studied using thermal gravimetric analysis (TGA). Filler interaction and chemical crosslinking was monitored using Fourier-transform infrared spectroscopy (FTIR) and film morphology were observed with field emission scanning electron microscopy (FESEM). Water uptake analysis, water contact angle and conductivity tests are also carried out. The results showed that when the GNP was incorporated at fixed CNF content, it was found to enhance the nanocomposite film, its mechanical, thermal and water behavior properties as supported by morphology and water uptake. Nanocomposite film with 0.5 wt.% GNP shows the highest improvement in term of tensile strength, Young's modulus, thermal degradation and water behavior. As the GNP loading increases, water uptake of the nanocomposite film was found relatively small (<1%). Contact angle test also indicates that the film is hydrophobic with addition of GNP. The conductivity properties of the nanocomposite film were not enhanced due to electrostatic repulsion force between GNP sheet and hard segment of WBPU. Overall, with addition of GNP, mechanical and thermal properties was greatly enhanced. However, conductivity value was not enhanced as expected due to electrostatic repulsion force. Therefore, ternary nanocomposite system is a suitable candidate for coating application.

Properties of Particleboard from Oil Palm Biomasses Bonded with Citric Acid and Tapioca Starch.

The study investigated the effects of the addition of starch on the properties of oil palm biomass particleboard bonded with citric acid. Three kinds of oil palm biomasses were used in this study for the fabrication of particleboard, namely, oil palm frond (OPF), oil palm trunk (OPT), and empty fruit bunch (EFB) particles. Citric acid and tapioca starch at the mixing ratios of 100:0, 87.5:12.5, and 75:25 were prepared at a 60% solid content. A 30% resin content based on the oven-dried weight of the oil palm biomass particles was used. The sprayed particles were pre-dried at 80 °C for 12 h before being hot-pressed at 180 °C and 4 MPa pressure for 10 min. The physical and mechanical properties of the particleboard were evaluated. The mixtures of citric acid and tapioca starch were characterized by thermogravimetric analysis (TGA). Thermal stability of citric acid was reduced after the addition of tapioca starch. The addition of 12.5% tapioca starch improved the bending strength of the particleboard but increased the thickness swelling slightly. All UF-bonded particleboard exhibited significantly inferior performance than that of citric-acid-bonded particleboard. Citric-acid-bonded particleboard maintained its original shape after being subjected to a cyclic-aging treatment, while the UF-bonded particleboard disintegrated half way through the treatment. The performance of EFB particleboard was significantly inferior to its OPT and OPF counterparts.

Physico-Mechanical and Biological Durability of Citric Acid-Bonded Rubberwood Particleboard.

This study investigated the effects of different citric acid content on the physico-mechanical and biological durability of rubberwood particleboard. Particleboards with density of 700 kg/m3 were produced with three different citric acid contents, namely 10, 15 and 20 wt%. Particleboards made from 10 wt% urea formaldehyde (UF) resin were served as control for comparison purposes. FTIR analysis was carried out and the formation of ester linkages between -OH on cellulose and carbonyl groups of citric acid was confirmed. The peak intensity increased along with increasing citric content, which indicated that a higher amount of ester linkages were formed at higher citric acid content. Citric acid-bonded particleboard had inferior physical properties (water absorption and thickness swelling) and mechanical properties (internal bonding strength, modulus of rupture and modulus of elasticity) compared to that of the UF-bonded particleboard. However, the performance of particleboard was enhanced with increasing citric acid content. Meanwhile, citric acid-bonded particleboard displayed significantly better fungal and termite resistance than UF-bonded particleboard owing to the acidic nature of citric acid. It can be concluded that citric acid is a suitable green binder for particleboard but some improvement is needed during the particleboard production process.