From:  Mechanisms and kinetics of drug release from lignin-based hydrogels: a review

 Synthesis methods, characteristics, and applications of lignin-based hydrogels.

Synthesis methodCrosslinking mechanismKey advantagesLimitationsApplicationsReferences
Free-radical polymerizationCovalent: lignin acts as a macro-initiator or macromonomer copolymerizing with vinyl monomers (e.g., acrylic acid, acrylamide).High gel strength, highly tunable swelling ratio (> 500 g/g), excellent reproducibility.Use of synthetic monomers, potential for toxic initiator residues, and complex purification.Super-absorbents, wastewater treatment.[16, 35, 37]
Chemical crosslinkingCovalent: reaction of lignin’s hydroxyl/carboxyl groups with crosslinkers, e.g., epichlorohydrin (EPI), glutaraldehyde, or PEG-diglycidyl ether.Simple process, high structural stability, direct use of lignin.Brittleness, potential toxicity of crosslinkers.Controlled-release matrices (fertilizers, drugs), adsorbents.[8, 47]
Enzymatic crosslinkingCovalent: oxidative enzymes (e.g., laccase, peroxidase) generate phenoxy radicals on lignin that undergo coupling.Green and sustainable process, high biocompatibility, mild reaction conditions.Slower kinetics, less control over network density, and high enzyme cost.Biomedical applications (tissue engineering, drug delivery).[19, 34, 44, 48]
Metal-ion coordinationPhysical: non-covalent coordination between lignin’s functional groups (e.g., catechol, carboxyl) and multivalent cations (Fe3+, Al3+, Zn2+).Injectable, self-healing, stimuli-responsive (pH, ions), reversible bonds.Mechanically softer; stability can be environment-dependent.Injectable drug depots, conductive composites, smart actuators.[22, 49]
Hydrogen bonding/host-guestPhysical: non-covalent interactions with polymers [e.g., polyvinyl alcohol (PVA), chitosan] or designed host-guest pairs (e.g., β-cyclodextrin-adamantane).Excellent biocompatibility, reversible and dynamic, shear-thinning.Generally weak mechanical properties, sensitive to temperature/pH.Wearable sensors, drug delivery carriers, and soft robotics.[21, 5052]