An Americium‐Containing Metal–Organic Framework: A Platform for Studying Transplutonium Elements

Ridenour, J. August; Surbella, Robert G.; Gelis, Artem V.; Koury, Daniel; Poineau, Frédéric; Czerwinski, Kenneth R.; Cahill, Christopher L.

doi:10.1002/ange.201909988

Cited by 6 publications

(12 citation statements)

References 60 publications

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“…There is a relative wealth (still less than 20 compounds) of structurally characterized americium–aquo bonds. The average water bond distance found in 1-Am is consistent with what is found in the literature such as [Am 2 (C 6 H 8 O 4 ) 3 (H 2 O) 2 ][(C 10 H 8 N 2 )] (2.469 Å), Am(TpyNO 2 )(NO 3 ) 3 )(H 2 O)·THF (TpyNO 2 = 4′-nitrophenyl terpyridyl; 2.467 Å), and [Am(H 2 O) 9 ][triflate] 3 (2.465–2.577 Å) …”

Section: Results and Discussionmentioning

confidence: 99%

Pronounced Pressure Dependence of Electronic Transitions for Americium Compared to Isomorphous Neodymium and Samarium Mellitates

et al. 2020

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The mellitate ion is relevant in spent nuclear fuel processing and is utilized as a surrogate for studying the interactions of f elements with humic acids. A wealth of different coordination modes gives the potential for diverse structural chemistry across the actinide series. In this study, an americium mellitate, 243Am2[(C6(COO–)6](H2O)8·2H2O (1-Am), has been synthesized and characterized using structural analysis and spectroscopy at ambient and elevated pressures. 1-Am was then compared to isomorphous neodymium (1-Nd) and samarium (1-Sm) mellitates via bond-length analysis and pressure dependence of their Laporte-forbidden f → f transitions. Results show that the pressure dependence of the f → f transitions of 1-Am is significantly greater than that observed in 1-Nd and 1-Sm, with average shifts of 21.4, 4.7, and 3.6 cm–1/GPa, respectively. This greater shift found in 1-Am shows further evidence that the 5f orbitals are more affected than the 4f orbitals when pressure is applied to isostructural compounds.

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Section: Results and Discussionmentioning

confidence: 99%

Pronounced Pressure Dependence of Electronic Transitions for Americium Compared to Isomorphous Neodymium and Samarium Mellitates

et al. 2020

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“…[1][2][3] At present, the uranium in radioactive wastewater is generally treated by the series of extraction, solidification, and landfill, inducing the massive abandonment of uranium resource. [4][5][6][7] In another aspect, uranium has a variety of valences ranging from +3 to +6 because radioactive wastewater was deposited on the MoS 2 nanosheets with precise mass loading and high selectivity for the common coexisting ions. In this case, the uranium was distributed on the sulfur edge (S-edge) sites and defect sites of MoS 2 in the existence form of U(IV) single atoms.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of Uranium Single Atom from Radioactive Wastewater for Enhanced Water Dissociation and Hydrogen Evolution

Liu

Tang

Liu

et al. 2022

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As a common nuclide in radioactive wastewater, uranium (U) is generally treated by landfill, which induces the massive abandonment of uranium resources. In this work, a pulse voltammetry method for the synthesis of U single atoms on MoS 2 (U/MoS 2 ) nanosheets from radioactive wastewater for the electrocatalytic alkaline hydrogen evolution reaction (HER) is reported. The mass loading of U single atoms is facilely controlled with high selectivity for coexisting ions in radioactive wastewater. In the electrolyte of 1 m of KOH, U/MoS 2 nanosheets with 5.2% of U single atoms exhibit relatively low overpotentials of 72 mV at 10 mA cm −2 . The mechanistic study reveals that the HER on U/MoS 2 includes the water dissociation on U single atoms to form OH* and H transfer from OH* to adjacent S-edge atoms. This procedure exhibits decreased activation energy for transition state in water dissociation and optimized Gibbs free energy for H* adsorption.

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“…Chemical exploration of the element americium (Z=95) in particular, suffers from this problem. This is highlighted by a recent search of the Cambridge Crystallographic Database, which contains over a million known crystal structures but only resulted in 55 known americium bearing compounds (Table S1, CSD version 2022.2.0) [1‐31] . For comparison, a search of uranium and plutonium resulted in 8,376 and 232 compounds, respectively.…”

Section: Introductionmentioning

confidence: 99%

“…Such materials can be defined as a specialized subclass of coordination polymers that potentially contain solvent‐accessible void spaces. Examples of transuranium metal‐organic frameworks (TRU‐MOFs) have recently begun to appear in the literature and in only the last four years are the actinides plutonium, [34] neptunium, [35,36] and americium [17] represented. For example, properties such as unusual local coordination and thermal stability, have been studied using these framework solids as hosts to immobilize actinides and study their behavior.…”

Section: Introductionmentioning

confidence: 99%

Insight into the Structural and Emissive Behavior of a Three‐Dimensional Americium(III) Formate Coordination Polymer

Nicholas

Arteaga

Ducati

et al. 2023

Chemistry A European J

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We report the structural, vibrational, and optical properties of americium formate (Am(CHO 2 ) 3 ) crystals synthesized via the in situ hydrolysis of dimethylformamide (DMF). The coordination polymer features Am 3 + ions linked by formate ligands into a three-dimensional network that is isomorphous to several lanthanide analogs, (e. g., Eu 3 + , Nd 3 + , Tb 3 + ). Structure determination revealed a nine-coordinate Am 3 + metal center that features a unique local C 3v symmetry. The metal-ligand bonding interactions were investigated by vibrational spectroscopy, natural localized molecular orbital calculations, and the quantum theory of atoms in molecules. The results paint a predominantly ionic bond picture and suggest the metal-oxygen bonds increase in strength from NdÀ O < EuÀ O < AmÀ O. The optical properties were probed using diffuse reflectance and photoluminescence spectroscopies. Notably, the rarely reported 5 D 1' ! 7 F 0' emission band is observed and dominates the emission spectrum. This behavior is unusual and is attributed to the C 3v coordination environment of the metal center.

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An Americium‐Containing Metal–Organic Framework: A Platform for Studying Transplutonium Elements

Cited by 6 publications

References 60 publications

Pronounced Pressure Dependence of Electronic Transitions for Americium Compared to Isomorphous Neodymium and Samarium Mellitates

Pronounced Pressure Dependence of Electronic Transitions for Americium Compared to Isomorphous Neodymium and Samarium Mellitates

Synthesis of Uranium Single Atom from Radioactive Wastewater for Enhanced Water Dissociation and Hydrogen Evolution

Insight into the Structural and Emissive Behavior of a Three‐Dimensional Americium(III) Formate Coordination Polymer

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