Phase evolution matters: How Fe(II) reshapes coprecipitate surfaces for enhanced U(VI) adsorption
Chaofei Zhang1, Yuan Chen2, Huiyang Mei3
1Northwest Institute of Eco-Environment and Resources, Chinese Academy of Sciences, Lanzhou 730000, China; Key Laboratory of Petroleum Resources Exploration and Evaluation, Gansu Province, Lanzhou 730000, China; University of Chinese Academy of Sciences, Beijing 100049, China.
Uranium (U(VI)) immobilization on iron (oxyhydr)oxides depends on iron ratios. Low Fe(II) density limits reductive immobilization, favoring adsorption pathways for uranium sequestration.
Area of Science:
- Environmental Science
- Geochemistry
- Materials Science
Background:
- Iron (oxyhydr)oxides are key for uranium sequestration.
- Uranium (VI) immobilization by Fe(II)/Fe(III) co-precipitates at moderate ratios needs clarification.
Purpose of the Study:
- Investigate phase evolution during Fe(II)/Fe(III) co-precipitation.
- Elucidate U(VI) immobilization mechanisms by these co-precipitates.
Main Methods:
- X-ray diffraction (XRD) and transmission electron microscopy (TEM) for phase analysis.
- Acid dissolution experiments to assess Fe(II) incorporation.
- Density functional theory (DFT) and spectroscopic analysis for reaction mechanisms.
Main Results:
- Low Fe(II)/Fe(III) ratio (1:50) maintained ferrihydrite phase; high ratio (1:10) transformed to goethite.
- Fe(II) incorporated into precipitate bulk, enhancing goethite surface reactivity for accelerated U(VI) immobilization.
- A reductive inert threshold for structural Fe(II) was identified between Fe(II)/Fe(III) ratios of 1:10 and 1:2.
Conclusions:
- Uranium immobilization is adsorption-dominated at low Fe(II) density, with limited reduction.
- Fe(II) speciation and availability critically influence uranium reduction.
- Findings provide a basis for predicting environmental uranium behavior.
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