Controllable sorption selectivity in zeolites is crucial for their application in catalysis, gas separation and ion-exchange. Whilst existing approaches to achieving sorption selectivity with natural zeolites typically rely on screening for specific geological deposits, here we develop partial interzeolite transformation as a straightforward and highly tuneable method to achieve sorption selectivity via forming dual-phase composites with simultaneous control of both phase-ratio and morphology. The dual-cation (strontium and caesium) exchange properties of a series of granular mordenite/zeolite P composites formed from a parent natural mordenite material are demonstrated in complex, industrially relevant multi-ion environments pertinent to nuclear waste management. The relative uptake of caesium and strontium is controlled via the extent of transformation: composites exhibit significantly increased ion-exchange affinity for strontium compared to both the parent mordenite and physical mixtures of mordenite/zeolite P phases with similar phase ratios. The composite with a 40 : 60 mordenite : zeolite P ratio composite achieves higher uptake rates than the natural clinoptilolite material currently used to decontaminate nuclear waste streams at the Sellafield site, UK. In situ X-ray image-guided diffraction experiments during caesium exchange demonstrate that the mordenite core retains rapid caesium uptake likely responsible for the unique ion-exchange chemistry achievable through the partial inter-zeolite transformation. These results offer a straightforward and controllable route to optimised zeolite functionality and a strategy to engineer composites from low-grade natural sources at low cost and with formulation advantages for industrial deployment.
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