The tris(carbonato)dioxouranium(VI) ion: A structural model for uranium 4f7/2, 5/2 X-ray photoelectron spectra satellite structures for oxide and oxygen coordination cores

Perry, Dale L.

doi:10.1016/j.vacuum.2014.10.013

Cited by 17 publications

(4 citation statements)

References 33 publications

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Section: Resultsmentioning

confidence: 99%

“…For Fe 3 O 4 @PDA-5-U, adsorbed U(VI) is evidenced by emergence of the U 4f signal, which shows two asymmetrical peaks assigned to U 4f 5/2 (392.5 eV) and U 4f 7/2 (382.0 eV) with a spin−orbit splitting of ∼10.5 eV (Figure S12b). 57 Besides, the characteristic U 4f 7/2 peak shows a binding energy of 382.0 eV, suggesting that the valence state of U(VI) remains unchanged after binding to PDA. 58 Deconvolution analysis of high-resolution XPS spectra affords an effective way to distinguish the specific chemical species or functional groups on solid surfaces, while revealing their interactions with metal ions.…”

Section: Environmental Science and Technologymentioning

confidence: 99%

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Performance and Mechanism of Uranium Adsorption from Seawater to Poly(dopamine)-Inspired Sorbents

et al. 2017

Environ. Sci. Technol.

197

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Developing facile and robust technologies for effective enrichment of uranium from seawater is of great significance for resource sustainability and environmental safety. By exploiting mussel-inspired polydopamine (PDA) chemistry, diverse types of PDA-functionalized sorbents including magnetic nanoparticle (MNP), ordered mesoporous carbon (OMC), and glass fiber carpet (GFC) were synthesized. The PDA functional layers with abundant catechol and amine/imine groups provided an excellent platform for binding to uranium. Due to the distinctive structure of PDA, the sorbents exhibited multistage kinetics which was simultaneously controlled by chemisorption and intralayer diffusion. Applying the diverse PDA-modified sorbents for enrichment of low concentration (parts per billion) uranium in laboratory-prepared solutions and unpurified seawater was fully evaluated under different scenarios: that is, by batch adsorption for MNP and OMC and by selective filtration for GFC. Moreover, high-resolution X-ray photoelectron spectroscopic and extended X-ray absorption fine structure studies were performed for probing the underlying coordination mechanism between PDA and U(VI). The catechol hydroxyls of PDA were identified as the main bidentate ligands to coordinate U(VI) at the equatorial plane. This study assessed the potential of versatile PDA chemistry for development of efficient uranium sorbents and provided new insights into the interaction mechanism between PDA and uranium.

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Section: Resultsmentioning

confidence: 99%

Section: Environmental Science and Technologymentioning

confidence: 99%

Performance and Mechanism of Uranium Adsorption from Seawater to Poly(dopamine)-Inspired Sorbents

et al. 2017

Environ. Sci. Technol.

197

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“…It is of importance for speciation of inorganic coordination compounds uranium with OH -, F -, NO 3 -, SO 4 2or CO 3 -, due to great reactivity of uranium in the gas phase and capability to form large number of stoichiometric and nonstoichiometric compounds. Same is valid for its reactivity in condense phase under experimental conditions (Ivanova and Spiteller 2014;Altmaier et al 2013;Perry 2015).…”

Section: Mass Spectrometric Methods Developmentmentioning

confidence: 89%

“…As it has been pointed out still in the abstract, the significance of the analytical objects studied herein concentrated in the fact that the UO 2 is among the most commonly used fuel din the nuclear reactors; however, the radiolysis of the water causing formation of the mentioned H 2 O 2 , OH Á , an relating species yielded to numerous non-stoichiometric compositions UO 2±x , each of which have different diffusion properties, meaning that the study of those compositions allows to understand the oxygen migration (Moore et al 2013;Yakub 2014;Berthinier et al 2013;Perry 2015). Such studies have significant impact to many interdisciplinary fields such as environmental analytical chemistry, radioanalytical chemistry, (bio)geochemistry and the fourth.…”

Section: Introductionmentioning

confidence: 99%

Environmental modeling of uranium interstitial compositions of non-stoichiometric oxides: experimental and theoretical analysis

Ivanova

Spiteller

2015

Environ Geochem Health

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Study of uranium interstitial compositions of non-stoichiometric oxides UO2+x (x ∈ 0.1-0.02) in gas and condense phases has been presented, using various soft-ionization mass spectrometric methods such as ESI-, APCI-, and MALDI-MS at a wide dynamic temperature gradient (∈ 25-300 °C). Linearly polarized vibrational spectroscopy has been utilized in order to assign unambiguously, the vibrational frequencies of uranium non-stoichiometric oxides. Experimental design has involved xUO2.66·yUO2.33, xUO2.66·yUO2.33/SiO2, xUO2.66·yUO2.33/SiO2 (NaOH) and SiO2/x'NaOH·y'UO2(NO3)2·6H2O, multicomponent systems (x = 1, y ∈ 0.1-1.0 and x' = 1, y' ∈ 0.1-0.6) as well as phase transitions UO2(NO3)2·6H2O → {U4O9(UO2.25)} → U3O7(UO2.33) → U3O8(UO2.66) → {UO3}, thus ensuring a maximal representativeness to real environmental conditions, where diverse chemical, geochemical and biochemical reactions, including complexation and sorption onto minerals have occurred. Experimental factors such as UV-irradiation, pH, temperature, concentration levels, solvent types and ion strength have been taken into consideration, too. As far as uranium speciation represents a challenging analytical task in terms of chemical identification diverse coordination species, mechanistic aspects relating incorporation of oxygen into UO 2+x form the shown full methods validation significantly impacts the field of environmental radioanalytical chemistry. UO2 is the most commonly used fuel in nuclear reactors around the globe; however, a large non-stoichiometric range ∈ UO1.65-UO2.25 has occurred due to radiolysis of water on UO2 surface yielding to H2O2, OH(·), and more. Each of those compositions has different oxygen diffusion. And in this respect enormous effort has been concentrated to study the potential impact of hazardous radionuclide on the environment, encompassing from the reprocessing to the disposal stages of the fuel waste, including the waste itself, the processes in the waste containers, the clay around the containers, and geological processes. In a broader sense, thereby, this study contributes to field of environmental analysis highlighting the great ability of various soft-ionization MS methods, particularly, MALDI-MS one, for direct assay of complex multicomponent heterogeneous mixtures at fmol-attomol concentration ranges, along with it the great instrumental features allowing, not only meaningful quantitative, but also structural information of the analytes, thus making the method indispensable for environmental speciation of radionuclides, generally.

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Erratum to: Environmental modeling of uranium interstitial compositions of non-stoichiometric oxides: experimental and theoretical analysis

Ivanova

Spiteller

2016

Environ Geochem Health

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The tris(carbonato)dioxouranium(VI) ion: A structural model for uranium 4f7/2, 5/2 X-ray photoelectron spectra satellite structures for oxide and oxygen coordination cores

Cited by 17 publications

References 33 publications

Performance and Mechanism of Uranium Adsorption from Seawater to Poly(dopamine)-Inspired Sorbents

Performance and Mechanism of Uranium Adsorption from Seawater to Poly(dopamine)-Inspired Sorbents

Environmental modeling of uranium interstitial compositions of non-stoichiometric oxides: experimental and theoretical analysis

Erratum to: Environmental modeling of uranium interstitial compositions of non-stoichiometric oxides: experimental and theoretical analysis

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