Clay minerals/sodium alginate/polyethylene hydrogel adsorbents control the selective adsorption and reduction of uranium: Experimental optimization and Monte Carlo simulation study

Jingjie Yang; Jianan Nie; Liang Bian; Jingmei Zhang; Mianxin Song; Fei Wang; Guocheng Lv; Li Zeng; Xiaobin Gu; Xin Xie; Peng Zhang; Qing Song

doi:10.1016/j.jhazmat.2024.133725

Clay minerals/sodium alginate/polyethylene hydrogel adsorbents control the selective adsorption and reduction of uranium: Experimental optimization and Monte Carlo simulation study

J Hazard Mater. 2024 Apr 15:468:133725. doi: 10.1016/j.jhazmat.2024.133725. Epub 2024 Feb 5.

Authors

Jingjie Yang¹, Jianan Nie², Liang Bian³, Jingmei Zhang², Mianxin Song², Fei Wang⁴, Guocheng Lv⁵, Li Zeng², Xiaobin Gu⁶, Xin Xie², Peng Zhang², Qing Song²

Affiliations

¹ State Key Laboratory of Environment-friendly Energy Materials, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China; Key Laboratory of Ministry of Education for Solid Waste Treatment and Resource Recycle, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China.
² Key Laboratory of Ministry of Education for Solid Waste Treatment and Resource Recycle, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China.
³ State Key Laboratory of Environment-friendly Energy Materials, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China; Key Laboratory of Ministry of Education for Solid Waste Treatment and Resource Recycle, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China; Tianfu Institute of Research and Innovation, Southwest University of Science and Technology, Chengdu 610299, Sichuan, China. Electronic address: bianliang@swust.edu.cn.
⁴ School of Energy and Environmental Engineering, Hebei University of Technology, Tianjin 300000, China.
⁵ School of Materials Science and Engineering, China University of Geosciences, Beijing 100000, China.
⁶ Guangzhou Institute of Energy Conversion, Chinese Academy of Science, Guangzhou 51000, China.

PMID: 38401209
DOI: 10.1016/j.jhazmat.2024.133725

Abstract

Clay minerals formations are potential geological barrier (host rocks) for the long-rerm storage of uranium tailing in deep geological repositories. However, there are still obstacles to the efficient retardation of uranium because of the competition between negatively charged regions at the clay minerals end face, surface and between layers, as well as low mineralization capacity. Herein, employing a simple method, we used sodium alginate (SA), an inexpensive natural polymer material, polyethylene (PE), and the natural clay minerals montmorillonite (Mt), nontronite (Nt), and beidellite (Bd) to prepare three hydrogel adsorbents, (denoted as Mt/PE-@SA, Nt/PE-@SA, and Bd/PE-@SA), respectively. The application of obtained hydrogel adsorbents further extends to uranium(VI) removal from aqueous. Due to the synergistic action of SA group and PE group, hydrogel adsorbents showed select adsorption and mineralization effect on uranium(VI), among which the maximum uranium(VI) adsorption capacity of Nt/PE-@SA was 133.3 mg·g^-1 and Mt/PE-@SA exhibited strong selectivity for uranium(VI) in the presence of coexisting metal ions. Cyclic voltammetry studies indicated the mitigation and immobilization of uranium species onto adsorbents by both reduction and mineralization. Besides, the synergistic adsorption of SA and PE on clay minerals was hypothesized, and the idea was supported by structure optimizations results from Monte Carlo dynamics simulation (MCD). Three obtained hydrogel adsorbents structural model was constructed based on its physicochemical characterization, the low energy adsorption sites and adsorption energies are investigated using MCD simulation. The simulation results show that obtained hydrogel adsorbents have a strong interaction with uranium(VI), which ensures the high adsorption capacity of those materials. Most importantly, this work demonstrates a new strategy for preparing mineral-based hydrogel adsorbents with enough stability and provides a new perspective for uranium(VI) removal in complex environment.

Keywords: Adsorption; Clay minerals; Monte Carlo dynamics simulation; Sodium alginate; Uranium(VI).