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Only small amounts of additives are needed to formulate one-component polyurethane (1C PUR) adhesives for various applications. The current study illuminates the effects of the formulation on the mechanical properties of pure adhesives, on the one hand, and their performance in bonded wood joints on the other. Tensile shear tests on bonded wood joints, tensile tests on adhesive films, and nanoindentation measurements in the interphase region of the bond were performed. Analyses by means of infrared, atomic force, and electron microscopy provided the explanatory basis for the results obtained. Additionally to laboratory made 1C PUR, unmodified commercial 1C PUR, melamine-urea-formaldehyde (MUF), and phenol-resorcinol-formaldehyde (PRF) were tested for comparison. The results obtained confirm that the mechanical properties of 1C PUR adhesives are significantly affected by their prepolymer composition. The adhesive formulation by means of additives, on the other hand, does not affect the mechanical properties but is to a large extent responsible for the bonding performance.

Filler materials are part and parcel for the adjustment of adhesives, in particular, their rheological and mechanical properties. Furthermore, the thermal stability of adhesives can be positively influenced by the addition of an expedient filler, with inorganic types common practice in most cases. In this study, one-component moisture-curing polyurethane adhesives for engineered wood products based on isocyanate prepolymers with different polymer-filled polyether polyols were investigated with regard to the filler's potential to increase the thermal stability of bonded wood joints. The property changes due to the addition of fillers were determined by means of mechanical tests on bonded wood joints and on pure adhesive films at different temperatures up to 200 C. Additional analyses by atomic force and environmental scanning electron microscopy advanced the understanding of the effects of the filler. The tested organic fillers, styrene acrylonitrile, a polyurea dispersion, and polyamide, caused increases in the cohesive strength and stiffness over the whole temperature range. However, the selected filler type was hardly important with regard to the tensile shear strength of the bonded wood joints at high temperatures, although the tensile strength and Young's modulus of the adhesive films differed over a wide range. Prepolymers with a lower initial strength and stiffness resulted in worse cohesion, in particular, at high temperatures. This disadvantage, however, could be compensated by means of the filler material. Ultimately, the addition of filler material resulted in optimized adhesive properties only in a well-balanced combination with the prepolymer used.

The reactivity of urethanes based on 1,6‐hexamethylene diisocyanate (HDI) and 4,4′‐methylene diphenyl diisocyanate (MDI) was investigated at temperatures between 190 °C and 235 °C. Diurethane model compounds end‐capped with either 1‐dodecanol (D‐core‐D) or 1‐hexadecanol (H‐core‐H) were mixed and annealed at high temperature. The core was either MDI or HDI. The transurethanization reaction was followed based on the formation of the compounds (H‐core‐D). The amount of H‐core‐D and of side products, which had formed after variable annealing times, were identified with 1H NMR, FTIR, SEC, and MALDI‐TOF. Transurethanization was considerably faster for MDI‐based urethanes than for HDI‐based urethanes. Only traces of side products were formed during annealing of MDI‐based urethanes, whereas a significant amount of allophanates was formed from HDI‐based urethanes under the same conditions. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 621–629

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