Benchmarking Uranyl Peroxide Capsule Chemistry in Organic Media

Neal, Harrison A.; Szymanowski, Jennifer; Fein, Jeremy B.; Burns, Peter C.; Nyman, May

doi:10.1002/ejic.201601219

Title: Benchmarking Uranyl Peroxide Capsule Chemistry in Organic Media

Journal Article · Tue Nov 29 00:00:00 EST 2016 · European Journal of Inorganic Chemistry

DOI:https://doi.org/10.1002/ejic.201601219· OSTI ID:1401247

Neal, Harrison A. ^[1];

^[2]; Fein, Jeremy B. ^[2]; Burns, Peter C. ^[2];

^[1]

Department of Chemistry Oregon State University Corvallis 97331 OR USA
Department of Civil &, Environmental Engineering &, Earth Sciences University of Notre Dame 46556 Notre Dame IN USA

Uranyl peroxide capsules are a recent addition to polyoxometalate (POM) chemistry. Ten years of development has ensued only in water, while transition metal POMs are commonly exploited in aqueous and organic media, controlled by counterions or ligation to render the clusters hydrophilic or hydrophobic. Here, new uranyl POM behavior is recognized in organic media, including (1) stabilization and immobilization of encapsulated hydrophilic countercations, identified by Li nuclear magnetic resonance (NMR) spectroscopy, (2) formation of new cluster species upon phase transfer, (3) extraction of uranyl clusters from different starting materials including simulated spent nuclear fuel, (4) selective phase transfer of one cluster type from a mixture, and (5) phase transfer of clusters from both acidic and alkaline media. The capsule morphology of the uranyl POMs renders accurate characterization by X‐ray scattering, including the distinction of geometrically similar clusters. Compositional analysis of the aqueous phase post‐extraction provided a quantitative determination of the ion exchange process that enables transfer of the clusters into the organic phase. Preferential partitioning of uranyl POMs into organic media presents new frontiers in metal ion behavior and chemical reactions in the confined space of the cluster capsules in hydrophobic media, as well as the reactivity of clusters at the organic/aqueous interface.

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Sponsoring Organization:: USDOE

OSTI ID:: 1401247

Journal Information:: European Journal of Inorganic Chemistry, Journal Name: European Journal of Inorganic Chemistry Vol. 2017 Journal Issue: 1; ISSN 1434-1948

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Cited by: 15 works

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References (48)

Sustained epoxidation of olefins by oxygen donors catalyzed by transition metal-substituted polyoxometalates, oxidatively resistant inorganic analogs of metalloporphyrins Hill, Craig L.; Brown, Robert B. Journal of the American Chemical Society, Vol. 108, Issue 3 https://doi.org/10.1021/ja00263a046	journal	February 1986
Elucidating Self-Assembly Mechanisms of Uranyl–Peroxide Capsules from Monomers Liao, Zuolei; Deb, Tapash; Nyman, May Inorganic Chemistry, Vol. 53, Issue 19 https://doi.org/10.1021/ic501587g	journal	September 2014
X-ray Studies of Interfacial Strontium–Extractant Complexes in a Model Solvent Extraction System Bu, Wei; Mihaylov, Miroslav; Amoanu, Daniel The Journal of Physical Chemistry B, Vol. 118, Issue 43 https://doi.org/10.1021/jp508430e	journal	October 2014
Hybrid Uranium-Oxalate Fullerene Topology Cage Clusters Ling, Jie; Wallace, Christine M.; Szymanowski, Jennifer E. S. Angewandte Chemie International Edition, Vol. 49, Issue 40 https://doi.org/10.1002/anie.201003197	journal	August 2010
Solution and Solid-State Structural Chemistry of Actinide Hydrates and Their Hydrolysis and Condensation Products Knope, Karah E.; Soderholm, L. Chemical Reviews, Vol. 113, Issue 2 https://doi.org/10.1021/cr300212f	journal	October 2012
Observation of a Rare Earth Ion–Extractant Complex Arrested at the Oil–Water Interface During Solvent Extraction Bu, Wei; Yu, Hao; Luo, Guangming The Journal of Physical Chemistry B, Vol. 118, Issue 36 https://doi.org/10.1021/jp505661e	journal	August 2014
B-α-[AsW ₉ O ₃₃ ] ⁹⁻ polyoxometalates incorporating hexanuclear uranium {U ₆ O ₈ }-like clusters bearing the U ^IV form or unprecedented mixed valence U ^IV /U ^VI involving direct U ^VI O–U ^IV bonding Duval, Sylvain; Sobanska, Sophie; Roussel, Pascal Dalton Transactions, Vol. 44, Issue 46 https://doi.org/10.1039/C5DT02932E	journal	January 2015
Solid-State Dynamics of Uranyl Polyoxometalates Alam, Todd M.; Liao, Zuolei; Zakharov, Lev N. Chemistry - A European Journal, Vol. 20, Issue 27 https://doi.org/10.1002/chem.201402351	journal	May 2014
Closing Uranyl Polyoxometalate Capsules with Bismuth and Lead Polyoxocations Renier, Olivier; Falaise, Clément; Neal, Harrison Angewandte Chemie International Edition, Vol. 55, Issue 43 https://doi.org/10.1002/anie.201607151	journal	September 2016
Micelle-mediated separation and cloud-point extraction Paleologos, Evangelos K.; Giokas, Dimosthenis L.; Karayannis, Miltiades I. TrAC Trends in Analytical Chemistry, Vol. 24, Issue 5 https://doi.org/10.1016/j.trac.2005.01.013	journal	May 2005
Onionlike Hybrid Assemblies Based on Surfactant-Encapsulated Polyoxometalates Li, Haolong; Sun, Hang; Qi, Wei Angewandte Chemie International Edition, Vol. 46, Issue 8 https://doi.org/10.1002/anie.200603934	journal	February 2007
Structural study of trivalent lanthanide and actinide complexes formed upon solvent extraction Gannaz, Beno?t; Antonio, Mark R.; Chiarizia, Renato Dalton Transactions, Issue 38 https://doi.org/10.1039/b609492a	journal	January 2006
Polyoxometalate-based functional nanostructured films: Current progress and future prospects Liu, Shaoqin; Tang, Zhiyong Nano Today, Vol. 5, Issue 4 https://doi.org/10.1016/j.nantod.2010.05.006	journal	August 2010
A Highly Transparent and Luminescent Hybrid Based on the Copolymerization of Surfactant-Encapsulated Polyoxometalate and Methyl Methacrylate Li, H.; Qi, W.; Li, W. Advanced Materials, Vol. 17, Issue 22 https://doi.org/10.1002/adma.200500893	journal	November 2005
The Key Role of U ₂₈ in the Aqueous Self-Assembly of Uranyl Peroxide Nanocages Falaise, Clément; Nyman, May Chemistry - A European Journal, Vol. 22, Issue 41 https://doi.org/10.1002/chem.201602130	journal	August 2016
Toward Nanodevices: Synthesis and Characterization of the Nanoporous Surfactant-Encapsulated Keplerate (DODA) ₄₀ (NH ₄ ) ₂ [(H ₂ O) _n ⊂Mo ₁₃₂ O ₃₇₂ (CH ₃ COO) ₃₀ (H ₂ O) ₇₂ ] Volkmer, Dirk; Du Chesne, Alexander; Kurth, Dirk G. Journal of the American Chemical Society, Vol. 122, Issue 9 https://doi.org/10.1021/ja992350v	journal	March 2000
Anisotropic ionic liquids built from nonmesogenic cation surfactants and Keggin-type polyoxoanions Jiang, Yunxia; Liu, Shuxia; Li, Shujun Chemical Communications, Vol. 47, Issue 37 https://doi.org/10.1039/c1cc13721b	journal	January 2011
Neodymium uranyl peroxide synthesis by ion exchange on ammonium uranyl peroxide nanoclusters Blanchard, F.; Ellart, M.; Rivenet, M. Chemical Communications, Vol. 52, Issue 20 https://doi.org/10.1039/C5CC09527A	journal	January 2016
Processing used nuclear fuel with nanoscale control of uranium and ultrafiltration Wylie, Ernest M.; Peruski, Kathryn M.; Prizio, Sarah E. Journal of Nuclear Materials, Vol. 473 https://doi.org/10.1016/j.jnucmat.2016.02.013	journal	May 2016
Binary Superlattices from {Mo ₁₃₂ } Polyoxometalates and Maghemite Nanocrystals: Long-Range Ordering and Fine-Tuning of Dipole Interactions Breitwieser, Romain; Auvray, Thomas; Volatron, Florence Small, Vol. 12, Issue 2 https://doi.org/10.1002/smll.201502127	journal	November 2015
Actinyl Peroxide Nanospheres Burns, Peter C.; Kubatko, Karrie-Ann; Sigmon, Ginger Angewandte Chemie, Vol. 117, Issue 14 https://doi.org/10.1002/ange.200462445	journal	March 2005
Water Radiolysis: Influence of Oxide Surfaces on H2 Production under Ionizing Radiation Le Caër, Sophie Water, Vol. 3, Issue 1 https://doi.org/10.3390/w3010235	journal	February 2011
Role of Ammonium Ions in the Formation of Ammonium Uranyl Peroxides and Uranyl Peroxo-oxalates Blanchard, Florent; Ellart, Marine; Rivenet, Murielle Crystal Growth & Design, Vol. 16, Issue 1 https://doi.org/10.1021/acs.cgd.5b01090	journal	November 2015
Purex process Starks, J. B. https://doi.org/10.2172/5220059	report	January 1977
Rapid Self-Assembly of Uranyl Polyhedra into Crown Clusters Sigmon, Ginger E.; Burns, Peter C. Journal of the American Chemical Society, Vol. 133, Issue 24 https://doi.org/10.1021/ja2013449	journal	June 2011
Evolution of Actinyl Peroxide Clusters U ₂₈ in Dilute Electrolyte Solution: Exploring the Transition from Simple Ions to Macroionic Assemblies Li, Dong; Simotwo, Silas; Nyman, May Chemistry - A European Journal, Vol. 20, Issue 6 https://doi.org/10.1002/chem.201303266	journal	January 2014
Molecular Probe Location in Reverse Micelles Determined by NMR Dipolar Interactions Crans, Debbie C.; Rithner, Christopher D.; Baruah, Bharat Journal of the American Chemical Society, Vol. 128, Issue 13 https://doi.org/10.1021/ja0583721	journal	April 2006
The U28 Nanosphere: What's Inside? Nyman, May; Rodriguez, Mark A.; Alam, Todd M. European Journal of Inorganic Chemistry, Vol. 2011, Issue 14 https://doi.org/10.1002/ejic.201001355	journal	March 2011
Chemical equilibria in the UO22+–H2O2–F−/OH− systems and possible solution precursors for the formation of [Na6(OH2)8]@[UO2(O2)F]2418− and [Na6(OH2)8]@[UO2(O2)OH]2418− clusters Zanonato, Pier Luigi; Di Bernardo, Plinio; Fischer, Andreas Dalton Transactions, Vol. 42, Issue 28 https://doi.org/10.1039/c3dt50837d	journal	January 2013
Closing Uranyl Polyoxometalate Capsules with Bismuth and Lead Polyoxocations Renier, Olivier; Falaise, Clément; Neal, Harrison Angewandte Chemie, Vol. 128, Issue 43 https://doi.org/10.1002/ange.201607151	journal	September 2016
Alkali–metal ion coordination in uranyl( vi ) poly-peroxo complexes in solution, inorganic analogues to crown-ethers. Part 2. Complex formation in the tetramethyl ammonium-, Li ⁺ -, Na ⁺ - and K ⁺ -uranyl( vi )–peroxide–carbonate systems Zanonato, Pier Luigi; Szabó, Zoltán; Vallet, Valerie Dalton Transactions, Vol. 44, Issue 37 https://doi.org/10.1039/C5DT01710F	journal	January 2015
Mixed-Valent Uranium(IV,VI) Diphosphonate: Synthesis, Structure, and Spectroscopy Diwu, Juan; Albrecht-Schmitt, Thomas E. Inorganic Chemistry, Vol. 51, Issue 8 https://doi.org/10.1021/ic300391p	journal	March 2012
Hybrid Uranium-Oxalate Fullerene Topology Cage Clusters Ling, Jie; Wallace, Christine M.; Szymanowski, Jennifer E. S. Angewandte Chemie, Vol. 122, Issue 40 https://doi.org/10.1002/ange.201003197	journal	August 2010
Clusters of Actinides with Oxide, Peroxide, or Hydroxide Bridges Qiu, Jie; Burns, Peter C. Chemical Reviews, Vol. 113, Issue 2 https://doi.org/10.1021/cr300159x	journal	October 2012
The Anderson–Evans polyoxometalate: From inorganic building blocks via hybrid organic–inorganic structures to tomorrows “Bio-POM” Blazevic, Amir; Rompel, Annette Coordination Chemistry Reviews, Vol. 307 https://doi.org/10.1016/j.ccr.2015.07.001	journal	January 2016
On the Origin of the Cation Templated Self-Assembly of Uranyl-Peroxide Nanoclusters Miró, Pere; Pierrefixe, Simon; Gicquel, Mickaël Journal of the American Chemical Society, Vol. 132, Issue 50 https://doi.org/10.1021/ja1053175	journal	December 2010
Irena : tool suite for modeling and analysis of small-angle scattering Ilavsky, Jan; Jemian, Peter R. Journal of Applied Crystallography, Vol. 42, Issue 2 https://doi.org/10.1107/S0021889809002222	journal	February 2009
Onionlike Hybrid Assemblies Based on Surfactant-Encapsulated Polyoxometalates Li, Haolong; Sun, Hang; Qi, Wei Angewandte Chemie, Vol. 119, Issue 8 https://doi.org/10.1002/ange.200603934	journal	February 2007
Single Crystal Growth and Structural Characterization of a Novel Mixed-Valent Ternary Uranium Oxide, K8U7O24 Read, Cory M.; Smith, Mark D.; zur Loye, Hans-Conrad Journal of Chemical Crystallography, Vol. 44, Issue 11-12 https://doi.org/10.1007/s10870-014-0555-x	journal	October 2014
Highly oxidation resistant inorganic-porphyrin analog polyoxometalate oxidation catalysts. 1. The synthesis and characterization of aqueous-soluble potassium salts of .alpha.2-P2W17O61(Mn+.cntdot.OH2)(n-10) and organic solvent soluble tetra-n-butylammonium salts of .alpha.2-P2W17O61(Mn+.cntdot.Br)(n-11) (M = Mn3+,Fe3+,Co2+,Ni2+,Cu2+) Lyon, David K.; Miller, Warren K.; Novet, Thomas Journal of the American Chemical Society, Vol. 113, Issue 19 https://doi.org/10.1021/ja00019a018	journal	September 1991
Self-Assembly of Organic−Inorganic Hybrid Amphiphilic Surfactants with Large Polyoxometalates as Polar Head Groups Zhang, Jie; Song, Yu-Fei; Cronin, Leroy Journal of the American Chemical Society, Vol. 130, Issue 44 https://doi.org/10.1021/ja805644a	journal	November 2008
Recovery of Uranium from Wet Phosphoric Acid by Solvent Extraction Processes Beltrami, Denis; Cote, Gérard; Mokhtari, Hamid Chemical Reviews, Vol. 114, Issue 24 https://doi.org/10.1021/cr5001546	journal	November 2014
Probing protein fine structures by wide angle solution X-ray scattering Zhang, R.; Thiyagarajan, P.; Tiede, D. M. Journal of Applied Crystallography, Vol. 33, Issue 3 https://doi.org/10.1107/S0021889800001345	journal	June 2000
The First Structural and Spectroscopic Characterization of a Neptunyl Polyoxometalate Complex Gaunt, Andrew J.; May, Iain; Helliwell, Madeleine Journal of the American Chemical Society, Vol. 124, Issue 45 https://doi.org/10.1021/ja028005e	journal	November 2002
Dynamics of Uranyl Peroxide Nanocapsules Nyman, May; Alam, Todd M. Journal of the American Chemical Society, Vol. 134, Issue 49 https://doi.org/10.1021/ja308673f	journal	November 2012
Reverse micelles as microreactors Pileni, M. P. The Journal of Physical Chemistry, Vol. 97, Issue 27 https://doi.org/10.1021/j100129a008	journal	July 1993
Actinyl Peroxide Nanospheres Burns, Peter C.; Kubatko, Karrie-Ann; Sigmon, Ginger Angewandte Chemie International Edition, Vol. 44, Issue 14 https://doi.org/10.1002/anie.200462445	journal	March 2005
Interaction of sulfur dioxide with heteropolyanions in nonpolar solvents. Evidence for complex formation Katsoulis, Dimitris E.; Tausch, Valerie S.; Pope, Michael T. Inorganic Chemistry, Vol. 26, Issue 1 https://doi.org/10.1021/ic00248a045	journal	January 1987

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