Room temperature synthesis of UO2+x nanocrystals and thin films via hydrolysis of uranium(<scp>iv</scp>) complexes

Murillo, Jesse; Panda, Debiprasad; Chakrabarti, Subhananda; Hattori, Alex; Griego, Leonel; Chava, Venkata S. N.; Sreeprasad, T. S.; Ramana, C. V.; Fortier, Skye

doi:10.1039/d1qi01248g

Cited by 4 publications

(2 citation statements)

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“…Figure S10 shows an amplified area between 2 and 38 degrees of diffractograms presented in Figure S9. XRD diffractograms in Figure S10 confirm U 3 O 8 (001), UO 2 (111), and UO 2 (200), − validating Raman spectroscopy and XPS results. All peaks show a low intensity, constraining the resolution of other XRD uranium oxides peaks. − The small thickness of uranium oxide films requires a characterization through grazing-incidence X-ray diffraction (GIXRD).…”

Section: Resultssupporting

confidence: 67%

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Stable Uranium Oxide Under Atmospheric Conditions: An Electroplating Technique for U Film Fabrication at Boron-Doped Diamond Electrodes

Peña-Duarte,

Acevedo-González,

Lagle

et al. 2023

ACS Mater. Au

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An electrodeposition technique of low-enriched uranium onto boron-doped diamond (BDD) electrodes for uranium electro-assembling, sequestration, uranium electrowinning (as the electroextraction alternative), and future neutron detection applications has been developed. Our findings through physicochemical characterization and an in-depth XPS analysis show that the U/BDD system consists of a blend of uranium oxides with IV, V, and VI oxidation states. Results show that U5+ is present and stable under open atmospheric conditions. The U electrodeposition on BDD creates smooth surfaces, free of voids, with uniform deposition of homogeneous tiny particles of stable uranium oxides, instead of chunky particles, and uranium compound mixtures, like large fibers of the precursor uranyl. Our electrochemical method operates without high temperatures or hazardous compounds. Uranium corrosion and oxidation processes occur spontaneously and parallel to the electrochemical formation of metallic uranium on BDD electrode surfaces, with metallic uranium reacting with water, producing fine particles of UO2. This work represents the first attempt to create a surface of uranium oxides, where the film thickness can be controlled for future applications, e.g., improving sensitivity in neutron detection technologies. Our U electro-assembling method provides a sustainable strategy for uranium electro-recovery from nuclear wastes, immobilizing uranium as a storage method or as U-film fabrication (U/BDD) for future neutron detection applications. Besides, this work contributes to uranium-based technologies, improving them and providing a better understanding of their electrochemical properties, e.g., uranium redox processes, uranium oxides’ formation, and stability evaluation. These properties are of remarkable need for uranium-based target formation. The use of our U/BDD method is proposed as an environmental protocol to recover and immobilize uranium-235, and other fissile materials, from civil and defense wastes, contaminated systems, and stockpiles.

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Section: Resultssupporting

confidence: 67%

“…All peaks show a low intensity, constraining the resolution of other XRD uranium oxides peaks. 48 − 53 The small thickness of uranium oxide films requires a characterization through grazing-incidence X-ray diffraction (GIXRD). For future works, we recommend evaluating the U-based films by using GIXRD.…”

Section: Resultsmentioning

confidence: 99%

Stable Uranium Oxide Under Atmospheric Conditions: An Electroplating Technique for U Film Fabrication at Boron-Doped Diamond Electrodes

Peña-Duarte,

Acevedo-González,

Lagle

et al. 2023

ACS Mater. Au

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All‐in‐One: Photo‐Responsive Lanthanide‐Organic Framework for Simultaneous Sensing, Adsorption, and Photocatalytic Reduction of Uranium

Huang,

Li,

Mei

et al. 2024

Adv Funct Materials

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The selective removal and immobilization of uranyl ions from aqueous solutions is essential for the sustainable development of nuclear energy. Herein, a robust lanthanide‐organic framework material (IHEP‐24) is developed for simultaneous fluorescence sensing, selective adsorption, and photocatalytic reduction of uranium, integrating three different functions in one material. The confined space formed by the coordination assembly of viologen derivative ligands and metal‐oxygen clusters can act as precise recognition sites for uranyl, allowing IHEP‐24 to efficiently detect and capture uranyl ions. In addition, the presence of a viologen‐based radical ligand enables IHEP‐24 to a further photocatalytic reduction of the adsorbed uranyl to amorphous UO2. The mechanisms of adsorption and photocatalysis are revealed by batch experiments, photoelectrochemical characterizations, and theoretical calculations. This study provides a reference for the construction of robust multi‐functional MOF materials and also provides support for the deep removal and immobilization of radionuclides from aqueous solution.

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Colloidal stability and surface chemistry of aqueous tetravalent uranium nanoparticles: Effects of 4-nitrocatechol adsorption

Yoon,

Cha,

Choi

et al. 2023

Surfaces and Interfaces

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Room temperature synthesis of UO_2+x nanocrystals and thin films via hydrolysis of uranium(iv) complexes

Abstract: Methods for the straightforward, room temperature synthesis of UO2+x nanoparticles and thin films using solution processable, molecular uranium(iv) compounds is described.

Cited by 4 publications

References 62 publications

Stable Uranium Oxide Under Atmospheric Conditions: An Electroplating Technique for U Film Fabrication at Boron-Doped Diamond Electrodes

Stable Uranium Oxide Under Atmospheric Conditions: An Electroplating Technique for U Film Fabrication at Boron-Doped Diamond Electrodes

All‐in‐One: Photo‐Responsive Lanthanide‐Organic Framework for Simultaneous Sensing, Adsorption, and Photocatalytic Reduction of Uranium

Colloidal stability and surface chemistry of aqueous tetravalent uranium nanoparticles: Effects of 4-nitrocatechol adsorption

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Room temperature synthesis of UO2+x nanocrystals and thin films via hydrolysis of uranium(iv) complexes

Abstract: Methods for the straightforward, room temperature synthesis of UO2+x nanoparticles and thin films using solution processable, molecular uranium(iv) compounds is described.

Cited by 4 publications

References 62 publications

Stable Uranium Oxide Under Atmospheric Conditions: An Electroplating Technique for U Film Fabrication at Boron-Doped Diamond Electrodes

Stable Uranium Oxide Under Atmospheric Conditions: An Electroplating Technique for U Film Fabrication at Boron-Doped Diamond Electrodes

All‐in‐One: Photo‐Responsive Lanthanide‐Organic Framework for Simultaneous Sensing, Adsorption, and Photocatalytic Reduction of Uranium

Colloidal stability and surface chemistry of aqueous tetravalent uranium nanoparticles: Effects of 4-nitrocatechol adsorption

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Room temperature synthesis of UO_2+x nanocrystals and thin films via hydrolysis of uranium(iv) complexes