Non‐Hydrothermal In Situ Synthesis of Ultra‐High and Radiation‐Resistant NaA Zeolite Microspheres for Cs ⁺ and Sr ²⁺ Remediation

Abstract Designing robust zeolites that integrate mechanical stability with irradiation resistance is pivotal yet challenging for nuclear wastewater treatment. Herein, a facile strategy enables binder‐free fabrication of NaA zeolite microspheres (GXU‐NaAs) for the first time via nonhydrothermal in situ synthesis using geopolymer technology with exceptional mechanical strength (compressive strength: 22.26 MPa, Vickers hardness: 395.48) without high pressure/temperature and secondary molding. The unique structure of GXU‐NaAs with cubic NaA zeolite embedded in an amorphous aluminosilicate matrix enables mechanical properties surpassing most traditional Na‐zeolites. Notably, GXU‐NaAs retains 99% of compressive strength and 99% adsorption capacity for Sr 2+ and Cs + after 500 KGy γ irradiation, outperforming conventional zeolites, which have the potential to maintain excellent stability in nuclear environments. GXU‐NaAs also exhibits excellent dynamic adsorption effect and adsorption cycling performance for Sr 2+ and Cs + with maximum adsorption capacities of 76.16 and 238.10 mg g −1 , maintaining excellent removal effect for Sr 2+ and Cs + in natural seawater. Density functional theory verifies the adsorption mechanism of Cs + and Sr 2+ on GXU‐NaAs. This work pioneers an advanced synthesis of high‐strength zeolite while providing a dual‐functional material for nuclear wastewater efficient remediation—simultaneously addressing mechanical stability and irradiation resistance in radionuclide capture challenges.