High‐Efficiency PFOA Removal by Microstructure‐Engineered Ultrathin Amphiphilic Mesoporous Reduced Graphene Oxide@Silica

Adsorption is a primary remediation strategy for per‐ and polyfluoroalkyl substances (PFAS) in aquatic systems. However, cost‐effective inorganic adsorbents typically underperform compared to expensive organic counterparts. Herein, we report a simple, scalable synthesis of an amphiphilic, ultrathin mesoporous adsorbent comprising reduced graphene oxide and mesoporous silica (rGO@mSiO 2 ). This architecture significantly enhances both mass transfer and binding affinity for perfluorooctanoic acid (PFOA). Owing to its tailored nanoscale amphiphilicity and reduced diffusion resistance, rGO@mSiO 2 rapidly achieves over 99% PFOA removal. It exhibits an ultrahigh adsorption capacity of 2421.78 mg g −1 , enabled by large pore channels facilitating efficient molecular packing. Furthermore, it demonstrates robust performance across diverse water matrices, excellent reusability, and a high affinity for short‐chain PFAS. Mechanistic studies reveal synergistic adsorption driven by hydrogen bonding, hydrophobic interactions, and pore‐confined self‐aggregation. These findings establish this purely inorganic adsorbent as a viable, scalable solution for PFAS remediation.