Synergistic immobilization and enhanced adsorption of Prussian blue via cellulose nanofiber/polyacrylamide dual-network interfacial engineering

Dual-network (DN) design is an effective means of constructing radionuclide-capturing aerogels with both high adsorption capacity and excellent stability. However, the fundamental role of DN structures in regulating the dispersion of encapsulated nanoparticles and the interfacial microenvironment remains unverified. Here, the synergistic immobilization and enhanced adsorption mechanism of CuFe-Prussian blue nanoparticles (CuFe-PB NPs) by a cellulose nanofiber/polyacrylamide dual network (CNF/PAM DN) were explored through experiments and simulations. The results show that PAM tightly encapsulates the PB/CNF composite via hydrogen bonding and physical entanglement, achieving a synergistic enhancement of the material's mechanical strength and structural stability. The resulting CNF/PAM DN - engineered PB aerogel (PB/CNF DN-A) retains 90% shape recovery after 100 compression cycles. Furthermore, molecular dynamics simulations elucidate that the DN structure provides ordered ion-transport channels and electrostatic synergy. Its unique “ion pre-enrichment” and “dehydration-assisted” effects effectively lower the energy barrier for Cs + removal within the hydration layer, enhancing the adsorption kinetics of Cs + . The optimized PB/CNF DN-A significantly reduced CuFe-PB NPs leakage and achieved a Cs + adsorption capacity of up to 403.9 mg/g within 50 min. In summary, this work deepens the understanding of interface-mediated interactions in multifunctional aerogels and provides a scalable platform for high-performance environmental remediation materials.