Insights into Stoichiometry Adjustments Governing the Performance of Flexible Foamed Polyurethane/Ground Tire Rubber Composites

Polyurethanes (PU) are widely applied in the industry due to their tunable performance adjusted by changes in the isocyanate index—stoichiometric balance between isocyanate and hydroxyl groups. This balance is affected by the incorporation of modifiers of fillers into the PU matrix and is especially crucial for PU foams due to the additional role of isocyanates—foaming of the material. Despite the awareness of the issue underlined in research works, the contribution of additives into formulations is often omitted, adversely impacting foams’ performance. Herein, flexible foamed PU/ground tire rubber (GTR) composites containing 12 different types of modified GTR particles differing by hydroxyl value (L(OH)) (from 45.05 to 88.49 mg KOH/g) were prepared. The impact of GTR functionalities on the mechanical, thermomechanical, and thermal performance of composites prepared with and without considering the L(OH) of fillers was assessed. Formulation adjustments induced changes in tensile strength (92–218% of the initial value), elongation at break (78–100%), tensile toughness (100–185%), compressive strength (156–343%), and compressive toughness (166–310%) proportional to the shift of glass transition temperatures (3.4–12.3 °C) caused by the additional isocyanates’ reactions yielding structure stiffening. On the other hand, formulation adjustments reduced composites’ thermal degradation onset due to the inferior thermal stability of hard segments compared to soft segments. Generally, changes in the composites’ performance resulting from formulation adjustments were proportional to the hydroxyl values of GTR, justifying the applied approach.