Changes in both formaldehyde legislations and voluntary requirements (e.g. Germany RAL) are currently the driving factors behind research on alternatives to amino-based adhesives; moreover, consumer interest in healthy and sustainable products is increasing in bio-based adhesives. Sources of formaldehyde emissions in wood-based panels as well as different emission test methods have been discussed, and the main focus of this review is on the research conducted on sustainable bio-based adhesive systems for wood panels. Lignin, tannin, protein, and starch have been evaluated as both raw materials and adhesive alternatives to existing amino-based thermosetting adhesives. Adhesion improving modifications of these bio-based raw materials as well as the available and experimental crosslinkers have also been taken into account.

Understanding the properties of any particular biorefinery or pulping residue lignin is crucial when choosing the right lignin for the right end use. In this paper, three different residual lignin types [supercritical water hydrolysis lignin (SCWH), ammonium lignosulfonate (A-LS), and sodium lignosulfonate (S-LS)] were evaluated for their chemical structure, thermal properties and water vapor adsorption behavior. SCWH lignin was found to have a high amount of phenolic hydroxyl groups and the highest amount of β-O-4 linkages. Combined with a low ash content, it shows potential to be used for conversion into aromatic or platform chemicals. A-LS and S-LS had more aliphatic hydroxyl groups, aliphatic double bonds and C=O structures. All lignins had available C₃/C₅positions, which can increase reactivity towards adhesive precursors. The glass transition temperature (T_g) data indicated that the SCWH and S-LS lignin types can be suitable for production of carbon fibers. Lignosulfonates exhibited considerable higher water vapor adsorption as compared to the SCWH lignin. In conclusion, this study demonstrated that the SCWH differed greatly from the lignosulfonates in purity, chemical structure, thermal stability and water sorption behavior. SCWH lignin showed great potential as raw material for aromatic compounds, carbon fibers, adhesives or polymers. Lignosulfonates are less suited for conversion into chemicals or carbon fibers, but due to the high amount of aliphatic hydroxyl groups, they can potentially be modified or used as adhesives, dispersants, or reinforcement material in polymers. For most value-adding applications, energy-intensive purification of the lignosulfonates would be required.Graphic

Tightening formaldehyde emission limits and the need for more sustainable materials have boosted research towards alternatives to urea-formaldehyde adhesives for wood-based panels. Lignin residues from biorefineries consist of a growing raw material source but lack reactivity. Two crosslinkers were tested for ammonium lignosulfonate (ALS)—bio-based furfuryl alcohol (FOH) and synthetic polymeric 4,4′-diphenylmethane diisocyanate (pMDI). The addition of mimosa tannin to ALS before crosslinking was also evaluated. The derived ALS adhesives were used for gluing 2-layered veneer samples and particleboards. Differential Scanning Calorimetry showed a reduction of curing temperature and heat for the samples with crosslinkers. Light microscopy showed that the FOH crosslinked samples had thicker bondlines and higher penetration, which occurred mainly through vessels. Tensile shear strength values of 2-layered veneer samples glued with crosslinked ALS adhesives were at the same level as the melamine reinforced urea-formaldehyde (UmF) reference. For particleboards, the FOH crosslinked samples showed a significant decrease in mechanical properties (internal bond (IB), modulus of elasticity (MOE), modulus of rupture (MOR)) and thickness swelling. For pMDI crosslinked samples, these properties increased compared to the UmF. Although the FOH crosslinked ALS samples can be classified as non-added-formaldehyde adhesives, their emissions were higher than what can be expected to be sourced from the particles.

The most common formaldehyde control method for wood panels in Europe, the perforator method, measures formaldehyde content, while most of the legal requirements in the world are based on emissions. Chamber methods typically used for emission measurements require too much time to reach steady state for factory quality control. The aim of this study was therefore to investigate whether emission values of particleboards measured one day after production would be usable for quality control purposes. The correlation between 1‐day and 7‐day emission values was determined using a dynamic microchamber (DMC). Three industrial board types that differed in density and emission levels were used for the evaluation. The online emission measuring equipment Aero‐laser AL4021 connected to the 1 m³ chamber was used to gain further information on the emission reduction behaviour of the different board types. Only the two particleboard types with higher densities showed good correlation between the 1‐day and 7‐day emissions. The overall results suggested that 1‐day emission values can be used for factory quality control purposes; however, if the initial 1‐day values are above the permitted level, extensive evaluation for each individual board type needs to be performed.