Highly selective adsorption and lattice process of cesium by cubic cyanide-based functional materials

Abstract

Cesium (Cs) is a byproduct of nuclear bombs, nuclear weapons testing, and nuclear fission in nuclear reactors. Cs can enter the human body through food or air and cause lasting damage. Highly efficient and selective removal of ¹³⁷Cs from low-level radioactive effluents (LLREs), which contain many radionuclides and dissolved heavy metal species, is imperative for minimizing LLRE volume, and facilitating their final disposal. Prussian blue analogs (PBAs) have received much attention as materials for the removal of radioactive Cs because of their affinity for adsorbing Cs⁺. In this study, an inexpensive and readily available cyanide-based functional material (PBA_Cu) exhibiting high efficiency and excellent selectivity toward Cs capture was designed through a facile low-temperature co-precipitation process. Nano-PBA_Cu, crystallizing in the cubic space group (Fm-3m (225)), has an average pore size of 6.53 nm; consequently, PBA_Cu can offer abundant atomic occupation sites for capturing and incorporating Cs. Here, the pseudo-second-order kinetic model and Langmuir model fitted well with the adsorption of Cs ⁺ on PBA_Cu, with a maximum capture capacity of 95.75 mg/g within 5 min, confirming that PBA_Cu could rapidly capture Cs ions. PBA_Cu strongly and selectively interacted with Cs even in a simulant containing large Na⁺, NH₄⁺, Ca²⁺, and Mg²⁺ ion concentrations in an aqueous solution. The process of Cs ⁺ adsorption by cyanide-based functional crystals was confirmed to involve the entry of Cs⁺ into cyanide-based functional crystals to replace K⁺ and finally achieve the lattice incorporation of Cs. The current results broaden the lattice theory of radionuclide Cs removal and provide a promising alternative for the immobilization of Cs from radioactive wastewater.

Keywords: Capture; Cesium; Incorporation; PBA(Cu); Radioactive wastewater.