Highly porous sensitive materials with well-defined structures and morphologies are extremely desirable for developing high-performance chemiresistive gas sensors. Herein, inspired by the classical alkaloid precipitant reaction, a robust and reliable active mesoporous nitrogen polymer sphere-directed synthesis method was demonstrated for the controllable construction of heteroatom-doped mesoporous tungsten oxide spheres. In the typical synthesis, P-doped mesoporous WO<sub>3</sub> monodisperse spheres with radially oriented channels (P-mWO<sub>3</sub>-R) were obtained with a diameter of ∼180 nm, high specific surface area, and crystalline skeleton. The in situ-introduced P atoms could effectively adjust the coordination environment of W atoms (W<sup>δ+</sup>-O<sub>v</sub>), giving rise to dramatically enhanced active surface-adsorbed oxygen species and unusual metastable ε-WO<sub>3</sub> crystallites. The P-mWO<sub>3</sub>-R spheres were applied for the sensing of 3-hydroxy-2-butanone (3H2B), a biomarker of foodborne pathogenic bacteria <i>Listeria monocytogenes</i> (<i>LM</i>). The sensor exhibited high sensitivity (<i>R</i><sub><i>a</i></sub>/<i>R</i><sub><i>g</i></sub> = 29 to 3 ppm), fast response dynamics (26/7 s), outstanding selectivity, and good long-term stability. Furthermore, the device was integrated into a wireless sensing module to realize remote real-time and precise detection of <i>LM</i> in practical applications, making it possible to evaluate food quality using gas sensors conveniently.
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