Incorporating pH/NIR responsive nanocontainers into a smart self-healing coating for a magnesium alloy with controlled drug release, bacteria killing and osteogenesis properties.

Magnesium (Mg)-based orthopedic implant materials can potentially be protected from deterioration using a protective polymer coating. However, this coating is susceptible to excessive corrosion and accidental scratches. Moreover, the inadequate bone integration and infections associated with bone implants present additional challenges that hinder their effective use. In this work, a spin-spray layer-by-layer (SSLbL) assembly technique was employed to develop a smart self-healing coating for Mg alloy WE43. This coating was based on paeonol-encapsulated nanocontainers (PMP) that were modified with a stimuli-responsive polydopamine (PDA). The leached paeonol could form a compact chelating layer when complexed with Mg2+ ions. Dynamic reversible hydrogen bonds were formed between assembly units, which ensured that the hybrid coating possessed rapid and cyclic self-healing properties. Under 808 nm near-infrared (NIR) laser irradiation, the self-healing coating exhibited antibacterial properties due to the synergistic effects of hyperthermia, reactive oxygen species (ROS), and paeonol. In addition, the incorporation of nanoparticles into the hybrid coating led to improvements in the cytocompatibility and osteogenic properties of the implant material. The smart coating enhanced alkaline phosphatase activity, extracellular matrix (ECM) mineralization, and the expression of osteogenic genes. This study presents a promising opportunity to explore the application of a smart self-healing coating for a Mg alloy. STATEMENT OF SIGNIFICANCE: Herein, we report a self-healing coating comprised of polyethyleneimine and nanocontainer-crosslinked hyaluronic acid to achieve drug-controlled release, antimicrobial activity, and osteogenesis performance. The formation of hydrogen bonds between HA and PEI facilitated the self-assembly process, thereby improving the coating's corrosion resistance and adhesion strength. The hybrid coating exhibited a rapid and cyclic self-healing activity due to paeonol and dynamic reversible bonds. The release of paeonol was controlled by pH and NIR stimuli owing to polydopamine modification. In vitro testing revealed that the hybrid coating achieved effective bacteria eradication through synergistic effects of hyperthermia, reactive oxygen species, and paeonol. Moreover, the smart coating was found to enhance alkaline phosphatase activity, extracellular matrix mineralization, and the expression of osteogenic genes.