Mechanically Robust Mesoporous UiO‐66‐NH2/Nanofibrous Aerogel for Organophosphonates Detoxification

Abstract There is a critical need for novel composite materials for high‐performance chemical filtration and detoxification of organophosphonates (OPs) and other harmful compounds found in nerve agents, pesticides, and industrial processes. In this work, rapid hydrolysis of OPs using high‐surface‐area zirconium‐based MOF‐aerogel composites is demonstrated. Using a unique surfactant‐templated solvothermal synthesis method, mesoporous UiO‐66‐NH 2 grown on the fibers within a polyacrylonitrile (PAN)/polyvinylpyrrolidone (PVP) nanofibrous sponge can produce a 3D MOF–polymer matrix with a specific surface area of up to 900 m 2 g −1 comp —almost 2X larger than the highest previously reported values while maintaining robust mechanical integrity. The mesoporous MOF promotes efficient diffusion, and the aerogel matrix provides a high‐surface‐area platform for spill containment. Unlike activated carbon, which adsorb OPs without degradation, the UiO‐66‐NH 2 ‐sponges hydrolyze OPs upon water contact, significantly reducing their toxicity. The MOF‐aerogel sponges withstand stresses up to 40 kPa under 70% strain are shown while maintaining exceptional catalytic efficiency, achieving a methyl paraoxon degradation half‐life of 3 min, compared to 15 min for similar microporous MOFs. This innovation accentuates the potential of mesoporous Zr‐MOF aerogels for advanced protection, filtration, and catalysis.