Tailoring abundant active-oxygen sites of Prussian blue analogues-derived adsorbents for highly efficient Yb(III) capture.

The removal of rare earth elements in mineral processing wastewater is highly desirable but still challenging. In this study, three bimetallic Prussian blue analogues (PBA) and six corresponding oxides are prepared by co-precipitation and calcination methods, and then utilized to adsorb aqueous Yb(III) solution. The results of XRD, SEM, BET, and XPS indicate the successful synthesis of all the adsorbents. Among them, three PBA-oxide samples (PBO-800) exhibit the superior adsorption capacities (˃250 mg/g). The adsorption processes of Yb(III) are in accordance with the pseudo-second-order kinetic model and Langmuir model, simultaneously showing the spontaneous and endothermic thermodynamics. Moreover, PBO-800 can be reused after alkaline solution regeneration with less than 10% degradation after five consecutive adsorption-desorption cycles. More importantly, PBO-800 exhibits the impressive separation selectivity of Yb(III) and most light rare earth ions (e.g., 5.51 of Yb/La, 4.03 of Yb/Pr), as well as the selectivity of Yb(III) and alkali metal ions (e.g., 300.5 of Yb/Na, 256.2 of Yb/Ca). According to the characterization analysis and DFT calculation, the adsorption mechanism of Yb(III) by PBO-800 is mainly attributed to the strong interaction between the abundant active-oxygen sites and Yb(III), and the significant electrostatic attraction. [Display omitted] • PBA-derived adsorbents with abundant active-oxygen sites are designed and fabricated. • Comparative study of PBA and PBA-oxides for adsorption of REEs is reported. • Mechanism reveals adsorption of Yb via surface complexation and electrostatic attraction. • Different affinity of Yb, light REEs and alkali metals benefits the selective separation. • Regenerated adsorbent is successfully reused for 5 times with less than 10% degradation. [ABSTRACT FROM AUTHOR]