Organic Fillers in Phenol-Formaldehyde Wood Adhesives

Veneer-based structural wood composites are typically manufactured using phenol-formaldehyde resols (PF) that are formulated with wheat flour extender and organic filler. Considering that this technology is several decades old, it is surprising to learn that many aspects of the formulation have not been the subject of detailed analysis and scientific publication. The effort described here is part of a university/industry research cooperation with a focus on how the organic fillers impact the properties of the formulated adhesives and adhesive bond performance. The fillers studied in this work are derived from walnut shell (Juglans regia), alder bark (Alnus rubra), and corn cob (furfural production) residue.

Alder bark and walnut shell exhibited chemical compositions that are typical for lignocellulosic materials, whereas corn cob residue was distinctly different owing to the high pressure steam digestion used in its preparation. Also, all fillers had low surface energies with dominant dispersive effects. Surface energy of corn cob residue was a little higher than alder bark and walnut shell, which were very similar.

All fillers reduced PF surface tension with effects greatest in alder bark and walnut shell. Surface tension reductions roughly correlated to the chemical compositions of the fillers, and probably resulted from the release of surface active compounds extracted from the fillers in the alkaline PF medium.

It was shown that viscoelastic network structures formed within the adhesive formulations as a function of shear history, filler type, and filler particle size. Relative to alder bark and walnut shell, the unique behavior of corn cob residue was discussed with respect to chemical composition.

Alder bark and walnut shell exhibited similar effects with a decrease of adhesive activation energy. However, corn cob reside caused much higher adhesive activation energy.

Alder bark exhibited significant particle size effects on fracture energy and bondline thickness, but no clear size effects on penetration. Regarding corn cob residue and walnut shell, particle size effects on fracture energy were statistically significant, but magnitude of the difference was rather small. Classified corn cob residue fillers all resulted in a similar bondline thickness (statistically no difference) that was different walnut shell.