Manganese monoxide (MnO), a versatile manganese oxide, is highly regarded for its potential to address heavy metal and radioactive contamination effectively. In this study, we investigated the adsorption mechanism of strontium nitrate solution on MnO crystal surfaces using molecular dynamics simulations. We examined the effects of adsorption and diffusion of ions and water molecules on three distinct MnO crystal surfaces. The results revealed significant differences in the adsorption capacities of Sr²⁺, NO₃⁻, and H₂O on the MnO crystal surfaces. The radial distribution function (RDF), the non-bond interaction energy (E_int), and mean square displacement (MSD) data indicate that Sr²⁺ exhibits the strongest interaction with the MnO (111) crystal surface. This results in a shift of Sr²⁺ from outer-sphere adsorption to inner-sphere adsorption. This strong interaction is primarily due to the increase in the number and prominence of non-bridging oxygen atoms on the MnO crystal surfaces.

To achieve efficient separation of Sr²⁺ under complex ionic-strength conditions, porous geopolymer particles (PGs) were used as a support to construct a K₂SbPO₆-loaded porous geopolymer composite, denoted as K₂SbPO₆@PGs, via in situ loading of one-dimensional K₂SbPO₆ by a high-temperature solid-state route. Its adsorption performance and mechanism were systematically compared with those of pristine PGs. Structural characterization (SEM/EDS, XRD, FTIR, XPS, and BET) confirmed that the K₂SbPO₆ crystalline phase was uniformly anchored onto the PGs framework while preserving interconnected mesoporous channels. K₂SbPO₆@PGs exhibited excellent Sr²⁺ removal over a wide pH range (3–12), with a removal efficiency of approximately 92% at pH 3, which was significantly higher than that of PGs (approximately 5%). The isotherm data were better fitted by the Sips model (R² = 0.982), and the maximum adsorption capacity reached 189.35 mg·g⁻¹ (theoretical qm = 201.14 mg·g⁻¹). Kinetic fitting showed that PGs followed the pseudo-first-order model, whereas K₂SbPO₆@PGs were better described by the pseudo-second-order model, indicating that chemical adsorption dominated the process through K⁺/Sr²⁺ exchange and surface complexation. Coexisting-ion experiments demonstrated strong resistance to monovalent ions, whereas Ca²⁺ and Mg²⁺ caused more pronounced competitive effects. The results indicate that PGs mainly provide interconnected mass-transfer pathways and granular structural support, whereas K₂SbPO₆ provides selective exchange sites with high affinity for Sr²⁺. The synergy between these two components endows the composite with good pH adaptability and enhanced adsorption performance and suggests its potential for subsequent continuous-flow separation studies.