Spray‐Coating of Catalytically Active MOF–Polythiourea through Postsynthetic Polymerization

A UiO‐66‐NCS MOF was formed by postsynthetic modification of UiO‐66‐NH₂. The UiO‐66‐NCS MOFs displays a circa 20‐fold increase in activity against the chemical warfare agent simulant dimethyl‐4‐nitrophenyl phosphate (DMNP) compared to UiO‐66‐NH₂, making it the most active MOF materials using a validated high‐throughput screening. The ?NCS functional groups provide reactive handles for postsynthetic polymerization of the MOFs into functional materials. These MOFs can be tethered to amine‐terminated polypropylene polymers (Jeffamines) through a facile room‐temperature synthesis with no byproducts. The MOFs are then crosslinked into a MOF–polythiourea (MOF–PTU) composite material, maintaining the catalytic properties of the MOF and the flexibility of the polymer. This MOF–PTU hybrid material was spray‐coated onto Nyco textile fibers, displaying excellent adhesion to the fiber surface. The spray‐coated fibers were screened for the degradation of DMNP and showed durable catalytic reactivity.