Unprecedented Humic Acid‐Resistant U(VI) Capture over Core–Shell Magnetic Mesoporous Aluminosilicate Microspheres

ABSTRACT The extraction of uranium from wastewater is critical for sustainable nuclear energy and environmental remediation, but is significantly challenged by the formation of stable uranium‐humic acid (HA) complexes, a widespread organic substance derived from plant and animal residues, severely limiting the efficiency of conventional adsorbents. To overcome this challenge, we designed magnetic mesoporous aluminosilicate core–shell microspheres (MMASS) with intrinsic high HA‐resistant via an interface emulsion assembly approach. The MMASS features superparamagnetic behavior, a high specific surface area (415 m 2 /g), tunable mesopores, and abundant Lewis acidic sites, enabling ultrahigh uranium uptake capacity (929 mg‐U/g) while maintaining exceptional resistance to HA interference. The high HA tolerance originates from highly exposed Lewis acidic Al sites, which preferentially binds U(VI) through inner‐sphere complexation to aluminum/silicon–O tetrahedra, forming a stable Al─O─U structure with a high binding energy (−8.98 eV) that significantly exceeds that of HA─U complexes (0.41 eV), as confirmed by DFT calculations and spectral analysis. Furthermore, the superparamagnetic core enables convenient magnetic separation and stable reuse over at least 18 cycles without loss of performance. This work provides a highly efficient and HA‐resistant adsorbent with strong potential for uranium extraction from complex real‐world wastewater.