Design of Nacre-Inspired 2D-MoS₂ Nanosheets Assembled with Mesoporous Covalent Organic Frameworks (COFs) for Smart Coatings

High loading capacity and smart release of inhibitors are the first and foremost characteristics of nanocontainers, which play a pivotal role in metal active corrosion protection. The present work explores the development of novel protective nanocontainers based on recently emerged covalent organic frameworks (COFs). These highly porous frameworks with large surface area, outstanding thermomechanical properties, low density, and ease of functionalization are used as nanocontainers. On the other hand, molybdenum disulfide (MoS₂), a state-of-the-art 2D layered compound with a sheetlike structure, was utilized thanks to its excellent barrier properties. However, these lamellar structures suffer a high agglomeration tendency in polymeric matrices. Therefore, we developed a novel hybrid nanocontainer, inspired by natural nacre, by an in situ growth of COF on MoS₂ to improve the stability and provide a high inhibitor loading capacity. The porous and nitrogen-rich structure of COF made it a good carrier to adsorb europium cations as inorganic inhibitors and release them on demand by pH changes to suppress the electrochemical reactions. The as-synthesized nanoplatforms were used as pH-responsive fillers in the epoxy resin. The nanocomposite coatings showed almost 50 kΩ cm² total resistance and high impedance values (10¹¹ Ω cm²) even after 77 days of immersion. Moreover, salt spray analysis depicted the smallest amount of rust and corrosion product after 31 days in the filled nanocomposite coating. Cathodic delamination and pull-off outcomes denoted that the filled coatings with the as-synthesized nanofiller showed the smallest cathodic delamination radius (3.41 mm) and lowest adhesion loss (24%) compared to the neat epoxy (7.55 mm and 46.7%). As such, the highly porous modified MoS₂ nanosheets are considered promising alternatives in a wide range of applications with anticorrosion properties.