Redox-active phytic acid-based self-assembled hybrid material for enhanced uranium adsorption from highly acidic solution

Abstract

Achieving efficient uranium adsorption from highly acidic wastewater is still considered challenging. Here, an inorganic-organic hybridized self-assembly material (rPFE-10) with redox activity was constructed by phytic acid (PA), ethylenediamine (EDA), and Fe(II) via a facile one-pot route, and further applied for U(VI) removal. In the static adsorption experiment, rPFE-10 achieved the maximum U(VI) adsorption capacity of 717.1 mg/g at the optimal pH of 3.5. It also performed preeminently in a highly acidic condition of pH = 1.0, with the highest adsorption capacity of 551.2 mg/g and an equilibrium time of 30 min. Moreover, rPFE-10 exhibited a pH-responsive adsorption selectivity for U(VI) and An-Ln (S(U(VI)) and S(An-Ln)), which increased to 69 % and 94 % respectively as pH decreased from 3.0 to 1.0. Additionally, the spectral analysis revealed a reconstruction mechanism induced by multiple synergistic adsorption, in which U(VI) exchange with EDA+/2+ and Fe2+/3+ and earned suitable coordination geometry and ligand environment to coordinate with PA (mainly P-OH), while partial U(VI) is reduced by Fe(II) in framework. This work not only highlights the facile strategy for enhanced U(VI) retention in highly acidic solution, but expands the potential application of supramolecular self-assembly material in treatment of nuclear wastewater.