Dynamic Metal-Phenolic Coordinated Hydrogel for Synergistic Photothermal/Chemodynamic Therapy against Biofilm-Infected Wounds and Real-Time Monitoring
Lixia Li, Zhonghao Zhao, Yuhang Gao, Xiaohe Jiang, Haimeng Liu, Xiaolu Guo, Xiaohua Huang, Li Zhou, Chanjuan Liu, Xing‐Can Shen
Abstract
The development of multifunctional hydrogel dressings integrating injectability, self-healing capability, tissue adhesion, multimodal antibacterial mechanisms, and real-time wound status monitoring remains a critical challenge for combating bacterial biofilms and accelerating wound healing. Herein, we present a dynamically cross-linked nanocomposite hydrogel (QCS-TA/LDH-panis) via Fe 3+ /Mn 2+ -mediated coordination between tannic acid (TA)-modified quaternized chitosan (QCS-TA) and polysulfonatoaniline-intercalated FeMn-layered double hydroxide (LDH-panis). The LDH-panis nanohybrids, synthesized through in situ polymerization of 3-sulfonatoaniline within FeMn-LDH interlayers, exhibit a near-infrared (NIR)-responsive photothermal effect (η = 64.3%) and pH/H 2 O 2 -activated peroxidase-like activity for biofilm-disrupting hydroxyl radical ( • OH) generation. Concurrently, the QCS-TA matrix enables a “capture-and-kill” mechanism via electrostatic interactions (quaternary ammonium groups) and bacterial affinity adhesion (catechol/pyrogallol moieties). Under near-infrared (NIR) irradiation, synergistic mild photothermal/chemodynamic therapy (mPTT/CDT) combined with contact-killing achieved >95% eradication of Staphylococcus aureus and Escherichia coli biofilms. Notably, the hydrogel’s conductivity enabled real-time monitoring of wound exudate and temperature fluctuation during the healing progression. In vivo evaluations confirmed accelerated infected wound regeneration (98.2% closure in 12 days) through biofilm elimination, inflammatory suppression, reepithelialization, and collagen deposition. This multifunctional hydrogel unifies dynamic adaptability, multimodal antibacterial therapy, and sensing intelligence, offering a promising strategy for the clinical management of biofilm-associated infection.