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Amino acid-based polymers combine biocompatibility, biodegradability, and structural
tunability, enabling their use in drug delivery, tissue engineering, and responsive soft materials.1 Among
various amino acid-derived building blocks, pyroglutamic acid (PGA), a cyclic lactam of glutamic acid,
remains relatively underexplored despite its inherent hydrogen (H)-bonding capability and structural
rigidity, which can be exploited to design advanced functional materials. In this regard, we developed
structurally tailored polymeric assemblies derived from PGA moiety and investigated their
multifunctional behavior. PGA-based homopolymers display pronounced thermoresponsive behavior,2
allowing reversible temperature-dependent phase transitions that modulate self-coacervation via H-
bonding interactions, ultimately resulting in liquid–liquid phase separation under suitable conditions.3
Such coacervate systems provided confined environments for efficient encapsulation of biomolecules.
Beyond encapsulation efficiency, modulation of the polymer backbone in PGA-based homopolymers
allows precise tuning of viscoelastic behavior, resulting in improved adhesive performance with higher
strength. Extending beyond homopolymer systems, this precursor has been judiciously incorporated
into block copolymer architectures, where it unlocks the potential for polymerization-induced self-
assembly (PISA).4 This methodology enables the in-situ formation of a diverse spectrum of
nanostructures with controlled morphology and hierarchical organization, thereby broadening the scope
of functional polymeric materials.5 Thus, this study establishes PGA-based polymers as a versatile
platform for designing multifunctional materials with integrated responsive and structural features. |