A multifunctional hydrogel that combines the properties
of pH-responsiveness
as well as controlled release holds enormous potential for antimicrobial
photodynamic therapy through the development of wound dressings and
coatings. Utilization of lignin (a biodegradable and cost-effective
biopolymer) could be advantageous as a sustainable alternative over
the conventional hydrogels for photodynamic therapy, which is an underexplored
area. In this work, the lignin-based hydrogel was developed, which
was found to have remarkable self-healing properties. Moreover, the
lignin-based photodynamic hydrogels designed via in situ and ex situ methods were found to be transparent
enough (through the variation of lignin concentration) to be utilized
for photodynamic therapy applications. The in situ method is an example of lignin hydrogel synthesis which is advantageous
as it saves multiple reaction steps of nanoparticle synthesis and
incorporation into the hydrogel. However, for the demonstration of
photodynamic effect, the lignin-based hydrogels were doped with a
photosensitizer (Rose Bengal, RB) and also with RB-conjugated lignin-derived
silver nanocomplexes (RB@L-AgNCs). The developed lignin-based nanocomposite
hydrogels were characterized through various methods including UV–vis
spectroscopy, HRTEM, BET, XRD, FESEM, rheology, and FTIR to determine
their material properties. Interestingly, the lignin hydrogels were
found to possess pH-responsive properties for controlled release of
the incorporated nanoagents. Antimicrobial photodynamic therapy studies
were performed using lignin-based nanocomposite hydrogels as well
as bare lignin hydrogels through utilization of a green laser for
a short time (3 min). Mechanistically, it was observed that the nanocomposite-doped
hydrogel worked much better as compared to the native lignin hydrogel
due to higher reactive oxygen species (ROS) generation. Furthermore,
the antimicrobial photodynamic activity of the developed lignin-based
nanocomposite hydrogels was validated through fluorescence microscopy
studies (live–dead cell imaging). These developed biodegradable
lignin-based nanocomposite hydrogels can be efficiently used for the
development of wound dressings and nanocoatings over various surfaces
for stimuli responsive antimicrobial effect.