MOF‐Derived Entropy‐Stabilized Quinary Alloy@Cellulose Aerogel for Ultrafast Tetracycline Degradation via PMS Activation

The persistent contamination of aquatic ecosystems by recalcitrant tetracycline antibiotics demands advanced catalytic systems beyond conventional oxidation methods. Here, a sustainable high‐entropy catalyst, FeMnCoZnCu@NCNP@CA is reported, comprising MOF‐derived multi‐metallic nanoparticles confined within a nitrogen‐doped carbon matrix and anchored on a 3D cellulose aerogel scaffold. The hybrid is obtained by pyrolyzing a quinary FeMnCoZnCu–NTA MOF precursor. This hierarchical design integrates several key features: high‐entropy stabilization to suppress phase segregation, N‐doping‐driven charge redistribution to enhance conductivity and active‐site density and multivalent redox coupling to promote reactive oxygen species generation (SO 4 • − , •OH, 1 O 2 ) and accelerate electron transfer. The confined carbon matrix effectively minimizes metal leaching (<0.1 ppm), while the aerogel macroporosity ensures rapid diffusion and enables >85% catalyst recovery. Under optimal conditions ([Catalyst] = 0.25 g L − 1 , [PMS] = 0.31 g L − 1 , pH = 3), FeMnCoZnCu@NCNP@CA achieves >98% tetracycline degradation within 15 min, exhibiting a rate constant (k = 0.070 ± 0.013 min − 1 ) that is 4.2 times higher than the mono‐metallic Fe@NCNP and surpasses di‐, tri‐ and tetra‐metallic analogues. This work highlights MOF‐derived high‐entropy hybrids as a promising platform for antibiotic remediation through the synergistic integration of multi‐metallic entropy, nitrogen doping, structural confinement and biomass aerogel engineering.