The aim of the present review is to summarize the current state of research in the field of sustainable bio-based adhesives used for production of eco-friendly wood composite materials. The article is focused mainly on the use of lignin, starch and tannins as raw materials and alternatives to the existing conventional adhesives. It is expected that increased amounts of biobased adhesives will be used in the production of wood composites in order to meet the current needs for development of sustainable and innovative materials which will make the wood-based panel industry more sustainable and lower its dependence on fossil fuels. However, there are still substantial challenges for the complete replacement of petroleum-based wood adhesives with biobased adhesives, mainly because of their relatively poor water resistance, low bonding strength and large natural variations due to different growing conditions. In this respect, fundamental research is still need in order to determine the factors for formulating bio-based adhesives with optimal properties and broaden their application in wood-based panel industry.

This review article aims to summarize the potential of using renewable natural resources, such as lignin and tannin, in the preparation of NIPUs for wood adhesives. Polyurethanes (PUs) are extremely versatile polymeric materials, which have been widely used in numerous applications, e.g., packaging, footwear, construction, the automotive industry, the lighting industry, insulation panels, bedding, furniture, metallurgy, sealants, coatings, foams, and wood adhesives. The isocyanate-based PUs exhibit strong adhesion properties, excellent flexibility, and durability, but they lack renewability. Therefore, this study focused on the development of non-isocyanate polyurethane lignin and tannin resins for wood adhesives. PUs are commercially synthesized using polyols and polyisocyanates. Isocyanates are toxic, costly, and not renewable; thus, a search of suitable alternatives in the synthesis of polyurethane resins is needed. The reaction with diamine compounds could result in NIPUs based on lignin and tannin. The research on bio-based components for PU synthesis confirmed that they have good characteristics as an alternative for the petroleum-based adhesives. The advantages of improved strength, low curing temperatures, shorter pressing times, and isocyanate-free properties were demonstrated by lignin- and tannin-based NIPUs. The elimination of isocyanate, associated with environmental and human health hazards, NIPU synthesis, and its properties and applications, including wood adhesives, are reported comprehensively in this paper. The future perspectives of NIPUs’ production and application were also outlined.

The potential of producing ecofriendly composites from industrial waste fibres, bonded with magnesium lignosulfonate, a lignin-based formaldehyde-free adhesive, was investigated in this work. Composites were produced in the laboratory using the following parameters: a hot press temperature of 210 °C, a pressing time of 16 min, and a 15% gluing content of magnesium lignosulfonate (on the dry fibres). The physical and mechanical properties of the produced composites were evaluated and compared with the European Standard (EN) required properties (EN 312, EN 622-5) of common wood-based panels, such as particleboards for internal use in dry conditions (type P2), load-bearing particleboards for use in humid conditions (type P5), heavy-duty load-bearing particleboards for use in humid conditions (type P7), and medium-density fibreboards (MDF) for use in dry conditions. In general, the new produced composites exhibited satisfactory mechanical properties: a bending strength (MOR) (18.5 N·mm−2) that was 42% higher than that required for type P2 particleboards (13 N·mm−2) and 16% higher than that required for type P5 particleboards (16 N·mm−2). Additionally, the modulus of elasticity (MOE) of composites (2225 N·mm−2) was 24% higher than that required for type P2 particleboards (1800 N·mm−2) and equivalent to the required MOE of MDF panels for use in dry conditions (2200 N·mm−2). However, these ecofriendly composites showed deteriorated moisture properties, i.e., 24 h swelling and 24 h water absorption, which were a distinct disadvantage. This should be further investigated, as modifications in the lignosulfonate formula used and/or production parameters are necessary.

The potential of using residual softwood fibers from the pulp and paper industry for producing eco-friendly, zero-formaldehyde fiberboard panels, bonded with calcium lignosulfonate (CLS) as a lignin-based, formaldehyde free adhesive, was investigated in this work. Fiberboard panels were manufactured in the laboratory by applying CLS addition content ranging from 8% to 14% (on the dry fibers). The physical and mechanical properties of the developed composites, i.e., water absorption (WA), thickness swelling (TS), modulus of elasticity (MOE), bending strength (MOR), as well as the free formaldehyde emission, were evaluated according to the European norms. In general, only the composites, developed with 14% CLS content, exhibited MOE and MOR values, comparable with the standard requirements for medium-density fiberboards (MDF) for use in dry conditions. All laboratory-produced composites demonstrated significantly deteriorated moisture-related properties, i.e., WA (24 h) and TS (24 h), which is a major drawback. Noticeably, the fiberboards produced had a close-to-zero formaldehyde content, reaching the super E0 class (≤1.5 mg/100 g), with values, ranging from 0.8 mg/100 g to 1.1 mg/100 g, i.e., equivalent to formaldehyde emission of natural wood. The amount of CLS adhesive had no significant effect on formaldehyde content.

The potential of producing eco-friendly, formaldehyde-free, high-density fiberboard (HDF) panels from hardwood fibers bonded with urea-formaldehyde (UF) resin and a novel ammonium lignosulfonate (ALS) is investigated in this paper. HDF panels were fabricated in the laboratory by applying a very low UF gluing factor (3%) and ALS content varying from 6% to 10% (based on the dry fibers). The physical and mechanical properties of the fiberboards, such as water absorption (WA), thickness swelling (TS), modulus of elasticity (MOE), bending strength (MOR), internal bond strength (IB), as well as formaldehyde content, were determined in accordance with the corresponding European standards. Overall, the HDF panels exhibited very satisfactory physical and mechanical properties, fully complying with the standard requirements of HDF for use in load-bearing applications in humid conditions. Markedly, the formaldehyde content of the laboratory fabricated panels was extremely low, ranging between 0.7–1.0 mg/100 g, which is, in fact, equivalent to the formaldehyde release of natural wood.

No abstract

No abstract

The pulp and paper industry generates substantial amounts of solid waste and wastewater, which contain waste fibres. The potential of using these recycled wood fibres for producing eco-friendly composites that were bonded with a formaldehyde-free adhesive (magnesium lignosulfonate) and their use in structural applications was evaluated in this study. Fibreboards were produced in the laboratory with a density of 720 kg·m−3 and 15% magnesium lignosulfonate gluing content, based on the dry fibres. The mechanical properties (bending strength, modulus of elasticity and internal bond strength), physical properties (thickness swelling and water absorption) and formaldehyde content were determined and compared with the European Standards requirements for wood-based panels. In general, the laboratory-produced panels demonstrated acceptable mechanical properties, such as bending strength (18.5 N·mm−2) and modulus of elasticity (2225 N·mm−2), which were higher than the minimum requirements for type P2 particleboards and equal to the requirements for MDF panels. The moisture properties, i.e., thickness swelling (24 h) and water absorption (24 h) significantly deteriorated. The free formaldehyde content of the laboratory-produced composites (1.1 mg/100 g) reached the super E0 grade (≤1.5 mg/100 g), which allowed for their classification as eco-friendly, low-emission wood-based composites. The L-type corner joints, made from the developed composites, demonstrated significantly lower bending capacity (from 2.5 to 6.5 times) compared to the same joints made from MDF panels. Nevertheless, the new eco-friendly composites can be efficiently utilised as a structural material in non-load-bearing applications.