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Developing tough adhesives with superior strength and ductility is challenging yet highly sought-after. In this work, we address a strategic approach to achieving diverse toughness and performance by meticulously harnessing weak electrostatic interactions. Two polyzwitterions (PZIs), derived from sulfobetaine methacrylate (SBMA), of different topologies: bottlebrush (BB-PSBMA) and linear (L-PSBMA), were designed. BB-PSBMA was synthesized using a rational "grafting-from" strategy, while L-PSBMA was prepared via atom transfer radical polymerization. Despite their architectural disparities, both PZIs demonstrated a comparable substantial lap-shear adhesion strength of ∼0.4 MPa. Intriguingly, the introduction of NaCl during adhesive preparation revealed contrasting adhesion behaviors. BB-PSBMA transitioned from a strong-brittle to strong-ductile adhesive upon the addition of 70 mM NaCl, evidenced by a 77.4% increase in the work of debonding, i.e., toughness. Further increases in NaCl concentration continued to impart the ductile properties to BB-PSBMA. Conversely, L-PSBMA adhesive predominantly transformed from strong-brittle to ductile regardless of the salt content. We propose a synergistic mechanism involving viscosity-governed optimal adhesion-cohesion balance and mechanical energy dissipation through sacrificial electrostatic association to elucidate the strong and ductile nature of the BB-PSBMA adhesive at 70 mM NaCl. Our findings emphasize the significance of precise control over architecture and salt concentration is necessary in constructing adhesives with enhanced toughness and performance.
Saha et al. (Mon,) studied this question.