Durable Physically Mixed Microporous and Mesoporous MOFs/Nanofiber Aerogel 3D Composites for Effective Toxic Gas Capture and Organophosphonate Detoxification

Abstract There is a critical need for innovative materials that offer efficient chemical filtration and detoxification of organophosphonates (OPs), pesticides, and other toxic industrial gases. In this study, a versatile method is introduced for fabricating 3D hierarchically porous mechanically stable nanofibrous aerogel (NFA)‐MOF composites with MOF mass fraction exceeding 80 wt.%, designed for enhanced detoxification. Mesoporous Zr‐MOF (UiO‐66‐NH 2 ), synthesized through a mild solvothermal process with cocamidopropyl betaine (CAPB) surfactant as a template, is combined with PAN/PVP nanofibrous dispersions to create composite NFAs. By adjusting CAPB concentration, MOF mesoporosity is tuned, achieving a maximum surface area of 1000 m 2 g −1 with 0.5 g CAPB. Composites containing UiO‐66‐NH 2 show effective hydrolysis of the DMNP simulant and degradation of chemical warfare agents (CWAs) such as soman (GD) and sulfur mustard (HD). The versatile mixing strategy is extended to incorporate microporous MOFs such as HKUST‐1 to enhance NFA functionality. Composites with HKUST‐1 effectively adsorb ammonia (NH 3 ), 2‐chloroethyl ethyl sulfide (CEES), and Cl 2 while mechanical and adhesion testing confirm that MOF loadings between 50 wt.% and 80 wt.% maintain excellent mechanical integrity. These multifunctional composite NFA offer significant potential as advanced materials for chemical defense, air purification, and environmental remediation, benefiting from a cost‐effective and environmentally friendly synthesis method.