Bioadhesive
membranes with controllable and reversible underwater
adhesion are desirable for several biomedical applications ranging
from biosensing, drug/therapeutic delivery, and tissue regeneration.
Here, we present dual soft mucosal and hard bone/enamel tissue adhesive
nanofiber membranes composed of chitosan and pectin derivatives for
pH-controlled delivery of antimicrobial peptides (AMPs) in the oral
cavity. Ex vivo testing with porcine esophagus (soft
mucosal mimic) indicated a 2-fold increase in the mucoadhesion of
chitosan membranes with 0.05 wt % oxidized pectin coating, while the
uncoated membranes exhibited 3–4-fold stronger adhesion to
hydroxyapatite discs (enamel/hard bone mimic) compared to the coated
membranes. The former is attributed to a synergistic interaction of
surface nanofiber topography, intermolecular hydrogen bonding, and
aldehyde–amine chemistry between surface polar groups and mucosal
proteins, while the latter may arise from electrostatic interactions
between cationic amines (−NH3
+) in chitosan
and anionic phosphates (−PO4
3–) in hydroxyapatite. Further, the dual hard–soft oral tissue
adhesive nanofiber membranes loaded with cationic amphipathic AMPs
(D-GL13K and IDR-1018) elicited pH-responsive AMP delivery and antimicrobial
action comparable to chlorhexidine (CHX) against oral streptococci.
Concurrently, the AMP loaded membranes were cytocompatible to both
soft epithelial tissue-derived human oral keratinocytes and hard calvarial
murine pre-osteoblast cells. We envision these membranes to function
as adhesive gingival grafts and guided bone regeneration (GBR) membranes
at the hard–soft tissue interface while simultaneously protecting
against oral infections.