journal article·2023-04Open access

Influence of groundwater composition on the reductive precipitation of U(VI) on corroding iron foil surfaces

N.L. Hansson, M. Saleh, P.L. Tam, S. Holgersson, K. Spahiu, C. Ekberg

Abstract

In order to assess the disposal of spent nuclear fuel in a deep geological nuclear waste repository, the interactions between U(VI) and corroded iron present in the canister material are of importance. It is important to correctly model the fate of the oxidatively dissolved uranium in order to correctly estimate radium releases from the canister in the long term. The release of radionuclides into the environment depends on the dissolution of the UO2 matrix which is dependent on the redox conditions at the fuel surface. The effect of metallic iron on the reduction of U(VI) was studied under anoxic conditions using synthetic groundwaters with different compositions, chosen to investigate the influence of calcium-uranyl-carbonato complexes on the thermodynamics and kinetics of U(VI) reduction on anoxically corroding iron. The corrosion products formed on the iron surface were investigated using SEM-EDS and XPS to identify elemental composition and oxidation states of uranium and iron on the surface. The iron foils efficiently reduced U(VI) to U(IV) causing its significant sorption and precipitation on the iron foil surfaces in the form of U(IV).
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Radioactive element chemistry and processing · Nuclear Materials and Properties · Groundwater flow and contamination studies

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (57)

Show source-provided references
1. King · 2001
2. Puigdomenech · 2001
3. On the fate of oxygen in a spent fuel emplacement drift in Opalinus Clay10.1016/j.apgeochem.2018.08.011 ↗
4. Badley · 2022
5. Svensk Kärnbränslehantering A.B., Technical Report TR-11-01 - Long-term safety for the final repository for spent nuclear fuel at Forsmark. Main report of the SR-Site project., (2011).
6. Pressure building during the early stages of gas production in a radioactive waste repository10.1016/S0022-3115(00)00184-7 ↗
7. The effect of temperature and fuel surface area on spent nuclear fuel dissolution kinetics under H2 atmosphere10.1016/j.jnucmat.2019.151981 ↗
8. Spent fuel corrosion and the impact of iron corrosion–the effects of hydrogen generation and formation of iron corrosion products10.1016/j.jnucmat.2020.152423 ↗
9. Effect of metallic iron on the oxidative dissolution of UO2 doped with a radioactive alpha emitter in synthetic Callovian-Oxfordian groundwater10.1016/j.gca.2017.08.043 ↗
10. Uranium removal from ground water using zero valent iron media10.1111/j.1745-6584.1999.tb01150.x ↗
11. Understanding the mechanism of uranium removal from groundwater by zero-valent iron using X-ray photoelectron spectroscopy10.1021/es970385u ↗
12. Reductive precipitation of uranium (VI) by zero-valent iron10.1021/es980010o ↗
13. Uranium precipitation in a permeable reactive barrier by progressive irreversible dissolution of zerovalent iron10.1021/es001204i ↗
14. Sorption and reduction of uranium (VI) on iron corrosion products under reducing saline conditions10.1524/ract.1996.74.special-issue.149 ↗
15. The reduction of U (VI) on corroded iron under anoxic conditions10.1524/ract.2002.90.9-11_2002.623 ↗
16. Nanoscale mechanism of UO2 formation through uranium reduction by magnetite10.1038/s41467-020-17795-0 ↗
17. Stable U (IV) complexes form at high-affinity mineral surface sites10.1021/es4047389 ↗
18. Reduction of U (VI) to U (IV) on the surface of magnetite10.1016/j.gca.2005.07.003 ↗
19. Reduction of uranium (VI) by mixed iron (II)/iron (III) hydroxide (green rust): formation of UO2 nanoparticles10.1021/es0208409 ↗
20. Surface catalysis of uranium (VI) reduction by iron (II)10.1016/S0016-7037(99)00265-3 ↗
21. Reduction of uranium (VI) by soluble iron (II) conforms with thermodynamic predictions10.1021/es2006012 ↗
22. Update on the chemical thermodynamics of uranium, neptunium, plutonium, americium and technetium, Nuclear Energy Agency Data Bank, Organization for Economic Co-operation
23. Speciation of uranium in seepage waters of a mine tailing pile studied by time-resolved laser-induced fluorescence spectroscopy (TRLFS)10.1524/ract.1996.74.special-issue.87 ↗
24. Uranyl (VI) carbonate complex formation: validation of the Ca2UO2 (CO3) 3 (aq.) species10.1524/ract.2001.89.8.511 ↗
25. Chemical speciation of uranium (VI) in marine environments: complexation of calcium and magnesium Ions with [(UO2)(CO3) 3] 4− and the effect on the extraction of uranium from seawater10.1002/chem.201403262 ↗
26. Grenthe · 2020
27. Calcium-uranyl-carbonato species kinetically limit U (VI) reduction by Fe (II) and lead to U (V)-bearing ferrihydrite10.1021/acs.est.9b05870 ↗
28. Inhibition of bacterial U (VI) reduction by calcium10.1021/es0210042 ↗
29. Effects of aqueous uranyl speciation on the kinetics of microbial uranium reduction10.1016/j.gca.2015.02.006 ↗
30. The effect of calcium on aqueous uranium (VI) speciation and adsorption to ferrihydrite and quartz10.1016/j.gca.2005.11.027 ↗
31. Impact of uranyl− calcium− carbonato complexes on uranium (VI) adsorption to synthetic and natural sediments10.1021/es902194x ↗
32. Agrenius · 2016
33. Kinetic energy discrimination in collision/reaction cell ICP-MS: theoretical review of principles and limitations10.1016/j.sab.2015.05.008 ↗
34. Rapid degradation of alkanethiol-based self-assembled monolayers on gold in ambient laboratory conditions10.1016/j.susc.2004.12.022 ↗
35. Summary of ISO/TC 201 Standard: VII ISO 15472: 2001—Surface chemical analysis—X-ray photoelectron spectrometers—calibration of energy scales10.1002/sia.1076 ↗
36. A step-by-step guide to perform x-ray photoelectron spectroscopy
37. XPS study of external α-radiolytic oxidation of UO2 in the presence of argon or hydrogen10.1016/j.jnucmat.2020.152604 ↗
38. XPS investigations on cesium uranates: mixed valency behaviour of uranium10.1016/S0022-3115(99)00146-4 ↗
39. Analysis of XPS spectra of Fe2+ and Fe3+ ions in oxide materials10.1016/j.apsusc.2007.09.063 ↗
40. XPS study of Fe(II)-Fe(III) (oxy)hydroxycarbonate green rust compounds10.1002/sia.2758 ↗
41. A consistent method for quantitative XPS peak analysis of thin oxide films on clean polycrystalline iron surfaces10.1016/S0169-4332(97)00167-0 ↗
42. XPS determination of uranium oxidation states10.1002/sia.3836 ↗
43. XPS study of uranium-containing sodium-aluminum-iron-phosphate glasses10.1016/j.jallcom.2017.04.025 ↗
44. Direct observation of pure pentavalent uranium in U 2 O 5 thin films by high resolution photoemission spectroscopy10.1038/s41598-018-26594-z ↗
45. X-ray photoelectron spectroscopy study of anodically oxidized SIMFUEL surfaces10.1016/j.electacta.2003.12.016 ↗
46. Investigation of multiplet splitting of Fe 2p XPS spectra and bonding in iron compounds10.1002/sia.1984 ↗
47. Effect of ultrasonic treatment on dispersibility of Fe3O4 nanoparticles and synthesis of multi-core Fe3O4/SiO2 core/shell nanoparticles10.1039/b505018a ↗
48. The effect of vacuum annealing of magnetite and zero-valent Iron nanoparticles on the removal of aqueous uranium
49. Combined in situ (ATR FT-IR) and ex situ (XPS) study of the ZnDTP-iron surface interaction10.1023/A:1024800900716 ↗
50. Uranium (VI) interaction with pyrite (FeS2): chemical and spectroscopic studies10.1524/ract.2006.94.9-11.651 ↗
51. Bedrock hydrogeochemistry Forsmark
52. A controlled, template-free, and hydrothermal synthesis route to sphere-like α-Fe 2 O 3 nanostructures for textile dye removal10.1039/C5RA26112K ↗
53. Solubility product of siderite (FeCO3) as a function of temperature (25–250 C)10.1016/j.chemgeo.2009.03.015 ↗
54. The role of green rust in the environment: a review10.1590/S1415-43662005000200021 ↗
55. The influence of aluminum on iron oxides. VI. The formation of Fe (II)-Al (III) hydroxy-chlorides,-sulfates, and-carbonates as new members of the pyroaurite group and their significance in soils10.1346/CCMN.1980.0280303 ↗
56. Description of input and examples for PHREEQC version 3—a computer program for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations
57. Finding and correcting calculation errors in PHREEQE