New Waterborne Polyurethane-Urea Synthesized with Ether-Carbonate Copolymer and Amino-Alcohol Chain Extenders with Tailored Pressure-Sensitive Adhesion Properties

New waterborne polyurethane-urea dispersions with adequate adhesion and cohesion properties have been synthesized by reacting isophorone diisocyanate, copolymer of ether and carbonate diol polyol and three amino-alcohols with different number of OH groups chain extenders using the prepolymer method. The waterborne polyurethane-urea dispersions were characterized by pH, particle-size distribution, and viscosity, and the polyurethane-urea films were characterized by attenuated total reflectance infrared (ATR-IR) spectroscopy, differential scanning calorimetry (DSC), thermal gravimetric analysis (TGA), and plate-plate rheology (temperature and frequency sweeps). Polyurethane-urea pressure-sensitive adhesives (PUU PSAs) were prepared by placing the waterborne polyurethane dispersions on polyethylene terephthalate (PET) films and they were characterized at 25 °C by creep test, tack and 180° peel test. The waterborne polyurethane-urea dispersions showed mean particle sizes between 51 and 78 nm and viscosities in the range of 58–133 mPa·s. The polyurethane-urea films showed glass transition temperatures (T(gs)) lower than −64 °C, and they showed a cross of the storage and loss moduli between −8 and 68 °C depending on the number of OH groups in the amino-alcohol chain extender. Different types of PUU PSAs (removable, high shear) were obtained by changing the number of OH groups in the amino-alcohol chain extender. The tack at 25 °C of the PUU PSAs varied between 488 and 1807 kPa and the 180° peel strength values ranged between 0.4 and 6.4 N/cm, and their holding times were between 2 min and 5 days. The new PUU PSAs made with amino-alcohol chain extender seemed very promising for designing environmentally friendly waterborne PSAs with high tack and improved cohesion and adhesion property.