Fibrous Zr‐MOF Nanozyme Aerogels with Macro‐Nanoporous Structure for Enhanced Catalytic Hydrolysis of Organophosphate Toxins

Metal–organic frameworks (MOFs) with Lewis acid catalytic sites, such as zirconium‐based MOFs (Zr‐MOFs), comprise a growing class of phosphatase‐like nanozymes that can degrade toxic organophosphate pesticides and nerve agents. Rationally engineering and shaping MOFs from as‐synthesized powders into hierarchically porous monoliths is essential for their use in emerging applications, such as filters for air and water purification and personal protection gear. However, several challenges still limit the production of practical MOF composites, including the need for sophisticated reaction conditions, low MOF catalyst loadings in the resulting composites, and poor accessibility to MOF‐based active sites. To overcome these limitations, a rapid synthesis method is developed to introduce Zr‐MOF nanozyme coating into cellulose nanofibers, resulting in the formation of processable monolithic aerogel composites with high MOF loadings. These composites contain Zr‐MOF nanozymes embedded in the structure, and hierarchical macro‐micro porosity enables excellent accessibility to catalytic active sites. This multifaceted rational design strategy, including the selection of a MOF with many catalytic sites, fine‐tuning the coating morphology, and the fabrication of a hierarchically structured monolithic aerogel, renders synergistic effects toward the efficient continuous hydrolytic detoxification of organophosphorus‐based nerve agent simulants and pesticides from contaminated water. A rapid synthesis method is developed to introduce Zr‐MOF nanozyme coating into cellulose nanofibers, resulting in the formation of processable macro‐micro porous aerogel composites with high metal–organic framework (MOF) loadings. The hierarchically structured MOF nanozymes monolithic aerogel enables excellent accessibility to catalytic active sites for fast and efficient hydrolytic detoxification of organophosphorus‐based nerve agent simulants and pesticides from contaminated water.