Aerogels Composed of Hierarchical Aramid Nanofibers and Carbon Nanotubes for Tetracycline Hydrochloride Removal

To address tetracycline (TCH) pollution, robust aramid nanofibers (ANF) were integrated with multi‐walled carbon nanotubes (CNT) via π–π conjugation and sol‐gel/freeze‐drying, forming ANFs/CNT aerogels. Systematic optimization of solid‐phase ratios and salt coagulation yielded Ca@ANFs/CNT. This composite achieved 94.6% removal of 20 mg/L TCH under ambient conditions, with a maximum adsorption capacity of 104.18 mg/g. It maintained high efficiency across pH 5–11 and resisted interference from common anions like Cl − and SO 4 2 − , though elevated CO 3 2 − concentrations and humic acid reduced performance via competitive adsorption and pH shifts. Kinetic/thermodynamic analyses confirmed chemical adsorption as the rate‐limiting step. Characterization (FT‐IR, XPS, and SEM) identified Ca 2 ⁺‐mediated chelation as the core mechanism, synergistically enhanced by electrostatic attraction, hydrogen bonding, π–π conjugation, and pore structure contributions. This study advances rational design of antibiotic‐capturing materials by clarifying structure‐function relationships, while demonstrating Ca@ANFs/CNT's practical viability for water purification. It establishes a paradigm for developing multifunctional adsorbents targeting aquatic emerging contaminants.