Trisilyl‐Functionalized Metal–Organic Framework Nanocrystallites for Synergistic Ultrafast Ppb‐Level Detection of Antibiotics and Organic Explosives

ABSTRACT Nitrofuran antibiotics and nitroaromatic compounds constitute critical organic pollutants and hazardous explosives, presenting significant ecological and public risks. The development of streamlined and efficient methods for their trace‐level detection remains a formidable challenge. Herein, we report the ultrarapid synthesis of metal–organic framework (MOF) nanocrystallites ( n SiTPE) within seconds, assisted by microwave. The trisilyl‐functionalized channels of n SiTPE serve as nanotraps, synergizing with the tetraphenyl ethene (TPE) units as built‐in fluorescent antennas. This dual‐function design endows n SiTPE with the state‐of‐the‐art sensitivity for nitroexplosives and nitroantibiotics (detection limits: 0.6–1.9 ppb) and ultrafast response times (< 1 s). Moreover, an n SiTPE‐based hydrogel enables smartphone‐integrated real‐time, quantitative, reusable, and on‐site detection, demonstrating exceptional portability. Mechanistic studies reveal that trisilyl groups modulate material hydrophobicity to drive analyte pre‐enrichment, while specific trisilyl‒nitro interactions create nanotraps within n SiTPE that capture ultratrace nitro analytes, thereby quenching the enhanced fluorescence from the TPE units. This work advances the rational design of high‐performance sensors for challenging environmental pollutants, offering new solutions for field‐deployable monitoring.