As
a primary molecular interaction governing unique phenomena found
in nature, hydrogen bonding (H-bonding) has played a significant role
in the design of functional polymeric materials. We herein present
the design and synthesis of poly(glycidoxy acetic acid) (PGA), which
involved H-bonding donor and acceptor moieties within a single repeating
unit of polyether for the precise control of the cooperative H-bonding
in polymer chains. The monomer-activated ring-opening polymerization
of a functional epoxide monomer, t-butyl glycidoxy
acetate, followed by hydrolysis, produced the desired PGA polymers
in a controlled manner. The high-level synergistic interplay between
the intermolecular and intramolecular H-bonding in the PGA chains
was demonstrated with pH-dependent self-association properties in
the solution state and stronger adhesion properties in the bulk state
compared with the conventional H-bonding mixture of poly(ethylene
oxide) and poly(acrylic acid). Furthermore, the molecular dynamics
simulations reveal the relative contributions of the respective H-bonding
interactions within the polymers in both the solution and the bulk
states, thereby highlighting their crucial role in the properties
of PGA. Finally, we anticipate the potential applicability of PGA
in biological and biomedical fields due to its excellent biocompatibility.
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