Abstract
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•Maximum U(VI) and Re(VII) uptake capacity of ZIF-8/PEI were 665.3 and 358.2 mg/g.•ZIF-8/PEI showed superior selectivity for U(VI) and Re(VII) under competitive ions.•U(VI) was coordinated with amino and terminal hydroxyl groups by XPS analysis.•Anion exchange dominated Re(VII) sequestration on ZIF-8/PEI by DFT calculation.
The simultaneously efficient removal of cationic and anionic radionuclides is an important and challenging topic for nuclear waste remediation as well as environmental protection. Herein, monoclinic ZIF-8 nanosheets modified with ethyleneimine polymer (denoted as ZIF-8/PEI) was achieved and used to determine the capture behaviors of both U(VI) oxycations and Re(VII) oxyanions from aqueous solution. ZIF-8/PEI assemblies showed a maximum U(VI) and Re(VII) uptake capacity of 665.3 (pH 5.0) and 358.2 mg/g (pH 3.5), respectively. Experimental, spectroscopic and theoretical calculation results directly unraveled that U(VI) adsorption onto ZIF-8/PEI assemblies was mainly ascribed to the coordination with abundant amino groups and weakly due to the Zn terminal hydroxyl groups, while anion exchange mechanism contributed predominantly to the Re(VII) sequestration. This work not only sheds light on the interaction mechanisms of simultaneous capture of U(VI) and Re(VII) but also highlights the versatile material design of cationic and anionic radionuclide immobilization in radioactive wastewater remediation.