In recent years, magnesium (Mg) alloys show a promising application in clinic as degradable biomaterials. Nevertheless, the poor corrosion resistance of Mg alloys is the main obstacle to their clinical application. Here we successfully seal the pores of plasma electrolytic oxidation (PEO) coating on AZ31 with Mg-Al layered double hydroxide (LDH) via hydrothermal treatment. PEO/LDH composite coating possess a two layer structure, an inner layer made up of PEO coating (~5 μm) and an outer layer of Mg-Al LDH (~2 μm). Electrochemical and hydrogen evolution tests suggest preferable corrosion resistance of the PEO/LDH coating. Cytotoxicity, cell adhesion, live/dead staining and proliferation data of rat bone marrow stem cells (rBMSCs) demonstrate that PEO/LDH coating remarkably enhance the cytocompatibility of the substrate, indicating a potential application in orthopedic surgeries. In addition, hemolysis rate (HR) test shows that the HR value of PEO/LDH coating is 1.10 ± 0.47%, fulfilling the request of clinical application. More importantly, the structure of Mg-Al LDH on the top of PEO coating shows excellent drug delivery ability.

Layered double hydroxides (LDHs) are widely studied to enhance corrosion resistance and biocompatibility of Mg alloys, which are promising bone implants. However, the influence of LDH coating on the osteointegration of Mg implants lacks of a systematic study. In this work, Mg-Al LDH coating was prepared on pure Mg via hydrothermal treatment. The as-prepared Mg-Al LDH coated Mg exhibited better in vitro and in vivo corrosion resistance than bare Mg and Mg(OH)2 coated Mg. In vitro culture of mouse osteoblast cell line (MC3T3-E1) suggested that Mg-Al LDH coated Mg was more favorable for its osteogenic differentiation. In vitro culture of HUVECs revealed that cells cultured in the extract of Mg-Al LDH coated Mg showed superior angiogenic behaviors. More importantly, the immune response of Mg-Al LDH coated Mg was studied by in vitro culturing murine-derived macrophage cell line (RAW264.7). The results verified that Mg-Al LDH coated Mg could induce macrophage polarize to M2 phenotype (anti-inflammatory). Furthermore, the secreted factor in the macrophage-conditioned culture medium of Mg-Al LDH group was more suitable for the bone differentiation of rat bone marrow stem cells (rBMSCs) and the angiogenic behavior of human umbilical vein endothelial cells (HUVECs). Finally, the result of femoral implantation suggested that Mg-Al LDH coated Mg exhibited better osteointegration than bare Mg and Mg(OH)2 coated Mg. With favorable in vitro and in vivo performances, Mg-Al LDH is promising as protective coating on Mg for orthopedic applications.