Structure of the hydrated dioxouranium(VI) ion in aqueous solution. An x-ray diffraction and proton NMR study

Aaberg, Maertha; Ferri, Diego; Glaser, Julius; Grenthe, Ingmar

doi:10.1021/ic00168a033

Cited by 130 publications

(127 citation statements)

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“…Work by Vachet and Callahan [14] has suggested that the nitrate anion, within gas-phase transition metal complexes, is primarily a bidentate ligand. The acceptance of three additional ligands by the uranyl-nitrate ion pair is consistent with a hypothesis that ESI produces a gasphase complex with a pentagonal bipyramidal conformation reminiscent of the structure of uranyl complexes in the solution phase [5][6][7][8][9][10][11]. The fact that the uranylhydroxide containing complex ion, as generated by ESI, also incorporated a maximum of 3 additional H 2 O ligands is therefore interesting.…”

Section: Discussionsupporting

confidence: 76%

“…The solution chemistry of uranium is dominated by the uranyl dication, UO 2 2ϩ , which is known to form complexes with a range of ligands [1]. Specific interaction with solvent will significantly influence the physico-chemical behavior of the uranyl ion and its complexes, and this has motivated investigations of complex composition and stability using infrared spectroscopy and extended X-ray absorption fine structure [5][6][7][8][9][10][11]. Unfortunately, explicit control over the interactions of solvent and nonsolvent ligands with the uranyl ion is difficult, which makes the study of species-dependent uranium behavior complicated.…”

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confidence: 99%

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Elucidation of the collision induced dissociation pathways of water and alcohol coordinated complexes containing the uranyl cation

Stipdonk

Anbalagan

Chien

et al. 2003

J. Am. Soc. Mass Spectrom.

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Multiple-stage tandem mass spectrometry was used to characterize the dissociation pathways for complexes composed of (1) the uranyl ion, (2) nitrate or hydroxide, and (3) water or alcohol. The complex ions were derived from electrospray ionization (ESI) ϩ . The abundance of the species was greater than expected based on previous experimental measurements of the (slow) hydration rate for UO 2 ϩ when stored in the ion trap. To account for the production of the hydrated product, a reductive elimination reaction involving reactive collisions with water in the ion trap is proposed. T he speciation and reactivity of uranium is a topic of sustained interest because species-dependent chemistry [1] controls processes ranging from nuclear fuel processing [2] to mobility and fate in the geologic subsurface [3,4]. The solution chemistry of uranium is dominated by the uranyl dication, UO 2 2ϩ , which is known to form complexes with a range of ligands [1]. Specific interaction with solvent will significantly influence the physico-chemical behavior of the uranyl ion and its complexes, and this has motivated investigations of complex composition and stability using infrared spectroscopy and extended X-ray absorption fine structure [5][6][7][8][9][10][11]. Unfortunately, explicit control over the interactions of solvent and nonsolvent ligands with the uranyl ion is difficult, which makes the study of species-dependent uranium behavior complicated. To gain a better understanding of the intrinsic interactions between different uranyl species and solvent, we have begun an investigation of uranyl-anion complexes in the gas phase using ion-trap mass spectrometry (IT-MS). Several recent reports have demonstrated that intrinsic metal and metal complex chemistry can be investigated by the (controlled) addition of reagent gas to an ion trap [12][13][14][15][16][17][18][19][20][21][22], or by way of the presence of H 2 O and other small molecule contaminants within the He bath gas used to collisionally cool ions and improve trapping efficiency [23][24][25]. The reactions of uranium ions in the gas phase have been the subject of several earlier investigations. Studies by , and by Schwarz and coworkers [30] have probed the reactions between U ϩ and UO ϩ and organic compounds such as alkanes and alcohols. Armentrout and Beauchamp [31] investigated the oxidation of U ϩ using small molecules such as O 2 , CO, CO 2 , COS, and

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Section: Discussionsupporting

confidence: 76%

mentioning

confidence: 99%

Elucidation of the collision induced dissociation pathways of water and alcohol coordinated complexes containing the uranyl cation

Stipdonk

Anbalagan

Chien

et al. 2003

J. Am. Soc. Mass Spectrom.

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“…weighted average of its two resonances, the acid resonance and the base resonance. 45 Therefore, when referring to those average sharp NMR peaks shown in Figures S2 and S3, free gluconate, gluconate and gluconic acid are used synonymously, unless specifically mentioned.…”

Section: Uo 2 (Gh 4 ) + Complex It Is Well Recognized That Solution mentioning

confidence: 99%

“…This is consistent with the structural results obtained previously for the fully hydrated uranyl ion. 45,46 The spectrum of solution XII (Fig. 7) shows a different pattern with a splitting in the O eq region, which suggests the O eq shell may be divided into two shells.…”

Section: Coordination Structures By Exafsmentioning

confidence: 99%

Complexation of Uranium(VI) by Gluconate in Acidic Solutions: a Thermodynamic Study with Structural Analysis

et al. 2009

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“…Then the investigation of uranyl species gives most basic information for other actinyl species investigation. Until now, so many experimental [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16] and theoretical approaches are performed for [UO 2 …”

Section: Introductionmentioning

confidence: 99%

Ab initio Quantum Chemical Study on Charge Distribution and Molecular Structure of Uranyl (VI) Species with Raman Frequency

Oda¹,

Aoshima²

2002

Journal of Nuclear Science and Technology

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Ab initio molecular orbital calculation was performed for uranyl (VI) monomer and dimer complexes with some water molecules and/or hydroxide ions. The Raman active frequencies were calculated for each complex after structural optimization in vacuum state, and investigated the molecular structure and the charge distribution. For uranyl monomer, the calculated Raman frequencies for uranyl with 5 or 6 water molecules show good agreement with experimental Raman frequencies for uranyl hydrates. On the contrary, the calculation underestimates the Raman frequency in case of hydroxide ions in uranyl complex. 4+ , and the theoretical Raman frequency and uranyl bond lengths have the good coincidence with those of experiments. The calculated uranyl bond length of dimer is slightly longer than that of monomer. Also, the charge of oxygen atom in uranyl shows larger change than that of uranium atom between dimer and monomer. And this charge distribution is mostly influenced by the charge donation of ligands. If only same ligands are surrounding, the number of ligands influenced this charge distribution.

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Structure of the hydrated dioxouranium(VI) ion in aqueous solution. An x-ray diffraction and proton NMR study

Cited by 130 publications

References 0 publications

Elucidation of the collision induced dissociation pathways of water and alcohol coordinated complexes containing the uranyl cation

Elucidation of the collision induced dissociation pathways of water and alcohol coordinated complexes containing the uranyl cation

Complexation of Uranium(VI) by Gluconate in Acidic Solutions: a Thermodynamic Study with Structural Analysis

Ab initio Quantum Chemical Study on Charge Distribution and Molecular Structure of Uranyl (VI) Species with Raman Frequency

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