Uranium mining and nuclear fuel production have led to significant U contamination. Past studies have focused on the bioreduction of soluble U(VI) to insoluble U(IV) as a remediation method. However, U(IV) is susceptible to reoxidation and remobilization when conditions change. Here, we demonstrate that a combination of adsorption and bioreduction of U(VI) in the presence of an organic ligand (siderophore desferrioxamine B, DFOB) and the Fe-rich clay mineral nontronite partially alleviated this problem. DFOB greatly facilitated U(VI) adsorption into the interlayer of nontronite as a stable U(VI)-DFOB complex. This complex was likely reduced by bioreduction intermediates such as the Fe(II)-DFOB complex and/or through electron transfer within a ternary Fe(II)-DFOB-U(VI) complex. Bioreduction with DFOB alone resulted in a mobile aqueous U(IV)-DFOB complex, but in the presence of both DFOB and nontronite U(IV) was sequestered into a solid. These results provide novel insights into the mechanisms of U(VI) bioreduction and the stability of U and have important implications for understanding U biogeochemistry in the environment and for developing a sustainable U remediation approach.

Download full-text PDF

Source
http://dx.doi.org/10.1021/acs.est.2c02047DOI Listing

Publication Analysis

Top Keywords

uvi adsorption
8
clay mineral
8
uvi
5
bioreduction
5
complex
5
siderophore dfob
4
dfob uvi
4
adsorption clay
4
mineral subsequent
4
subsequent reduction
4

Similar Publications

A strategically designed ternary nanohybrid (TNS-PDA/CNT), consisting of titanate nanosheet (TNS) and polydopamine-modified multiwalled carbon nanotube (PDA/CNT composite), was synthesized by the facile hydrothermal method and wet impregnation method for removal of U(VI) from aqueous solution and were characterized by transmission electron microscopy (TEM), scanning electron microscopy-energy-dispersive X-ray spectroscopy (SEM-EDS), X-ray diffraction (XRD), Fourier transform infrared (FT-IR), thermogravimetric analysis (TGA), Raman spectroscopy, Brunauer-Emmett-Teller (BET), and X-ray photoelectron spectroscopy (XPS). TNSs were introduced into the PDA/CNT composite, which effectively averted the agglomeration of the CNT and further exposed more adsorption sites. PDA thin layer exposing more active sites was conducive to enhance adsorption capacity and kinetic.

View Article and Find Full Text PDF

An Amidoxime-functionalized chitosan dual-network hydrogel: Enhanced uranium-water separation capacity.

Int J Biol Macromol

December 2024

Key Laboratory of Eco-Functional Polymer Materials of the Ministry of Education, Research Center of Gansu Military and Civilian Integration Advanced Structural Materials, College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou 730070, PR China.

The source and after treatment of uranium, a key aspect of its use as a nuclear fuel, had been a topic of intense debate among developers. Therefore, a novel antimicrobial amidoxime-functionalized chitosan/polyacrylamide dual network hydrogel (CP-AO) had been developed utilizing a straightforward methodology. The results demonstrated excellent adsorption capacity and selectivity for uranium extraction under varying conditions, the U(VI) removal was above 94 % when pH was 4.

View Article and Find Full Text PDF

Effects of EDTA and Bicarbonate on U(VI) Reduction by Reduced Nontronite.

Environ Sci Technol

December 2024

Center for Geomicrobiology and Biogeochemistry Research, State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Beijing 100083, China.

Widespread Fe-bearing clay minerals are potential materials capable of reducing and immobilizing U(VI). However, the kinetics of this process and the impact of environmental factors remain unclear. Herein, we investigated U(VI) reduction by chemically reduced nontronite (rNAu-2) in the presence of EDTA and bicarbonate.

View Article and Find Full Text PDF

How to Evaluate the Chemical Affinity of -OH and -COOH Functional Groups Toward U(VI).

Molecules

November 2024

School of Chemistry and Chemical Engineering, Yantai University, Yantai 264005, China.

Which functional group shows a stronger affinity for U(VI) and can be introduced into material to enhance selective enrichment? This is crucial for U(VI) capture material design and evaluation. Following these questions, we herein compared and analyzed bare graphene, graphene oxide (GO), and carboxylated graphene oxide (GO-COOH) through experimental and theoretical calculations. Experiments show that U(VI) adsorption on GO-COOH ( = 344.

View Article and Find Full Text PDF

Among all natural submicrosized phases, clay minerals are ubiquitous in soils and sedimentary rocks in nature as well as in engineered environments, and while clay minerals' adsorption properties have been studied extensively, their unique level of surface reactivity heterogeneities necessitates further investigation at the molecular level to understand and predict the influence of these heterogeneities on their macroscopic properties. In this study, we investigated the surface structures and desorption-free energies of U(VI) species (UO) and As(V) species (HAsO and HAsO) complexed at different edge surface reactive sites of a cis-vacant montmorillonite layer using first-principles molecular dynamics (FPMD). We show that U(VI) forms bidentate and tridentate complexes on montmorillonite edge surfaces, whereas As(V) monodentate complexes are the most stable.

View Article and Find Full Text PDF

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!