Flux crystal growth: a versatile technique to reveal the crystal chemistry of complex uranium oxides

Juillerat, Christian A.; Klepov, Vladislav V.; Morrison, Gregory; Pace, Kristen A.; zur Loye, Hans-Conrad

doi:10.1039/c8dt04675a

Title: Flux crystal growth: a versatile technique to reveal the crystal chemistry of complex uranium oxides

Journal Article · Tue Jan 01 00:00:00 EST 2019 · Dalton Transactions

DOI:https://doi.org/10.1039/c8dt04675a· OSTI ID:1566637

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Department of Chemistry and Biochemistry; Center for Hierarchical Wasteform Materials; University of South Carolina; Columbia; USA

This frontier article focuses on the use of flux crystal growth for the preparation of new actinide containing materials, reviews the history of flux crystal growth of uranium containing phases, and highlights the recent advances in the field. Specifically, we discuss how recent developments in f-element materials, fueled by accelerated materials discovery via crystal growth, have led to the synthesis and characterization of new families of complex uranium containing oxides, namely alkali/alkaline uranates, oxychlorides, oxychalcogenides, tellurites, molybdates, tungstates, chromates, phosphates, arsenates, vanadates, niobates, silicates, germanates, and borates. An overview of flux crystal growth is presented and specific crystal growth approaches are described with an emphasis on how and why they – versus some other method – are used and how they enable the preparation of specific classes of new materials.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Hierarchical Waste Form Materials (CHWM); Univ. of South Carolina, Columbia, SC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

DOE Contract Number:: SC0016574

OSTI ID:: 1566637

Journal Information:: Dalton Transactions, Vol. 48, Issue 10; ISSN 1477-9226

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

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Flux Synthesis, Crystal Structure, and Photoluminescence of a Heterometallic Uranyl-Europium Germanate with U═O–Eu Linkage: K ₄ [(UO ₂ )Eu ₂ (Ge ₂ O ₇ ) ₂ ] Liu, Shih-Pu; Chen, Meng-Ling; Chang, Bor-Chen Inorganic Chemistry, Vol. 52, Issue 7 https://doi.org/10.1021/ic302826u	journal	June 2012
Observation of an Unusual Uranyl Cation–Cation Interaction in the Strongly Fluorescent Layered Uranyl Phosphates Rb ₆ [(UO ₂ ) ₇ O ₄ (PO ₄ ) ₄ ] and Cs ₆ [(UO ₂ ) ₇ O ₄ (PO ₄ ) ₄ ] Juillerat, Christian A.; Moore, Emily E.; Besmann, Theodore Inorganic Chemistry, Vol. 57, Issue 7 https://doi.org/10.1021/acs.inorgchem.8b00302	journal	December 2017
Versatile Uranyl Germanate Framework Hosting 12 Different Alkali Halide 1D Salt Inclusions Juillerat, Christian A.; Moore, Emily E.; Morrison, Gregory Inorganic Chemistry, Vol. 57, Issue 18 https://doi.org/10.1021/acs.inorgchem.8b01729	journal	August 2018
Synthesis and structure of the new pentanary uranium( vi ) silicate, K ₄ CaUSi ₄ O ₁₄ , a member of a structural family related to fresnoite Morrison, Gregory; Smith, Mark D.; Tran, T. Thao CrystEngComm, Vol. 17, Issue 22 https://doi.org/10.1039/C5CE00504C	journal	January 2015
A Family of Layered Phosphates Crystallizing in a Rare Geometrical Isomer of the Phosphuranylite Topology: Synthesis, Characterization, and Computational Modeling of A ₄ [(UO ₂ ) ₃ O ₂ (PO ₄ ) ₂ ] (A = Alkali Metal) Exhibiting Intralayer Ion Exchange Juillerat, Christian A.; Moore, Emily E.; Kocevski, Vancho Inorganic Chemistry, Vol. 57, Issue 8 https://doi.org/10.1021/acs.inorgchem.8b00434	journal	March 2018
Flux Synthesis, Structure, Properties, and Theoretical Magnetic Study of Uranium(IV)-Containing A ₂ USi ₆ O ₁₅ (A = K, Rb) with an Intriguing Green-to-Purple, Crystal-to-Crystal Structural Transition in the K Analogue Morrison, Gregory; Ramanantoanina, Harry; Urland, Werner Inorganic Chemistry, Vol. 54, Issue 11 https://doi.org/10.1021/acs.inorgchem.5b00556	journal	May 2015
Formation of Open Framework Uranium Germanates: The Influence of Mixed Molten Flux and Charge Density Dependence in U-Silicate and U-Germanate Families Li, Haijian; Langer, Eike M.; Kegler, Philip Inorganic Chemistry, Vol. 57, Issue 17 https://doi.org/10.1021/acs.inorgchem.8b01781	journal	August 2018
Crystal chemistry of anhydrous Li uranyl phosphates and arsenates. II. Tubular fragments and cation–cation interactions in the 3D framework structures of Li6[(UO2)12(PO4)8(P4O13)], Li5[(UO2)13(AsO4)9(As2O7)], Li[(UO2)4(AsO4)3] and Li3[(UO2)7(AsO4)5O)] Alekseev, Evgeny V.; Krivovichev, Sergey V.; Depmeier, Wulf Journal of Solid State Chemistry, Vol. 182, Issue 11 https://doi.org/10.1016/j.jssc.2009.08.003	journal	November 2009
Crystal chemistry of anhydrous Li uranyl phosphates and arsenates. I. Polymorphism and structure topology: Synthesis and crystal structures of α-Li[(UO2)(PO4)], α-Li[(UO2)(AsO4)], β-Li[(UO2)(AsO4)] and Li2[(UO2)3(P2O7)2] Alekseev, Evgeny V.; Krivovichev, Sergey V.; Malcherek, Thomas Journal of Solid State Chemistry, Vol. 181, Issue 11 https://doi.org/10.1016/j.jssc.2008.07.028	journal	November 2008
Flux Growth of [NaK ₆ F][(UO ₂ ) ₃ (Si ₂ O ₇ ) ₂ ] and [KK ₆ Cl][(UO ₂ ) ₃ (Si ₂ O ₇ ) ₂ ]: The Effect of Surface Area to Volume Ratios on Reaction Products Morrison, Gregory; zur Loye, Hans-Conrad Crystal Growth & Design, Vol. 16, Issue 3 https://doi.org/10.1021/acs.cgd.5b01408	journal	January 2016
Molten salt flux synthesis and crystal structure of a new open-framework uranyl phosphate Cs3(UO2)2(PO4)O2: Spectroscopic characterization and cationic mobility studies Yagoubi, S.; Renard, C.; Abraham, F. Journal of Solid State Chemistry, Vol. 200 https://doi.org/10.1016/j.jssc.2013.01.013	journal	April 2013
Highly Distorted Uranyl Ion Coordination and One/Two-Dimensional Structural Relationship in the Ba ₂ [UO ₂ (TO ₄ ) ₂ ] (T = P, As) System: An Experimental and Computational Study Wu, Shijun; Kowalski, Piotr M.; Yu, Na Inorganic Chemistry, Vol. 53, Issue 14 https://doi.org/10.1021/ic500965v	journal	June 2014
K ₈ (K ₅ F)U ₆ Si ₈ O ₄₀ : An Intergrowth Uranyl Silicate Morrison, Gregory; Tran, T. Thao; Halasyamani, P. Shiv Inorganic Chemistry, Vol. 55, Issue 7 https://doi.org/10.1021/acs.inorgchem.6b00242	journal	March 2016
Understanding the Formation of Salt-Inclusion Phases: An Enhanced Flux Growth Method for the Targeted Synthesis of Salt-Inclusion Cesium Halide Uranyl Silicates Morrison, Gregory; Smith, Mark D.; zur Loye, Hans-Conrad Journal of the American Chemical Society, Vol. 138, Issue 22 https://doi.org/10.1021/jacs.6b03205	journal	May 2016
Complex Topology of Uranyl Polyphosphate Frameworks: Crystal Structures of α-, β-K[(UO2)(P3O9)] and K[(UO2)2(P3O10)] Alekseev, Evgeny V.; Krivovichev, Sergey V.; Depmeier, Wulf Zeitschrift für anorganische und allgemeine Chemie, Vol. 634, Issue 9 https://doi.org/10.1002/zaac.200700384	journal	August 2008
Further Insight into Uranium and Thorium Metaphosphate Chemistry and the Effect of Nd ³⁺ Incorporation into Uranium(IV) Metaphosphate : Actinide Metaphosphate Chemistry Yu, Na; Klepov, Vladislav V.; Neumeier, Stefan European Journal of Inorganic Chemistry, Vol. 2015, Issue 9 https://doi.org/10.1002/ejic.201403098	journal	February 2015
Flux versus Hydrothermal Growth: Polymorphism of A ₂ (UO ₂ )Si ₂ O ₆ (A = Rb, Cs) Morrison, Gregory; Smith, Mark D.; zur Loye, Hans-Conrad Inorganic Chemistry, Vol. 56, Issue 3 https://doi.org/10.1021/acs.inorgchem.6b02931	journal	January 2017
Flux Synthesis of Salt-Inclusion Uranyl Silicates: [K ₃ Cs ₄ F][(UO ₂ ) ₃ (Si ₂ O ₇ ) ₂ ] and [NaRb ₆ F][(UO ₂ ) ₃ (Si ₂ O ₇ ) ₂ ] Lee, Cheng-Shiuan; Wang, Sue-Lein; Chen, Yen-Hung Inorganic Chemistry, Vol. 48, Issue 17 https://doi.org/10.1021/ic901001n	journal	September 2009
Rubidium uranyl phosphates and arsenates with polymeric tetrahedral anions: Syntheses and structures of Rb4[(UO2)6(P2O7)4(H2O)], Rb2[(UO2)3(P2O7)(P4O12)] and Rb[(UO2)2(As3O10)] Alekseev, Evgeny V.; Krivovichev, Sergey V.; Depmeier, Wulf Journal of Solid State Chemistry, Vol. 182, Issue 8 https://doi.org/10.1016/j.jssc.2009.05.022	journal	August 2009
Solid-state syntheses and single-crystal characterizations of three tetravalent thorium and uranium silicates Jin, Geng Bang; Soderholm, L. Journal of Solid State Chemistry, Vol. 221 https://doi.org/10.1016/j.jssc.2014.10.018	journal	January 2015
Synthesis, structure, and optical properties of CsU2(PO4)3 Oh, George N.; Ringe, Emilie; Van Duyne, Richard P. Journal of Solid State Chemistry, Vol. 185 https://doi.org/10.1016/j.jssc.2011.10.007	journal	January 2012
Novel layered uranyl arsenates, Ag6[(UO2)2(As2O7)(As4O13)] and AI6[(UO2)2(AsO4)2(As2O7)] (AI–Ag and Na): first observation of a linear As4O136− anion and structure type evolution Alekseev, Evgeny V.; Krivovichev, Sergey V.; Depmeier, Wulf Journal of Materials Chemistry, Vol. 19, Issue 17 https://doi.org/10.1039/b818757f	journal	January 2009
Synthèse et structure du borouranate de lithium LiBUO5 Gasperin, M. Acta Crystallographica Section C Crystal Structure Communications, Vol. 46, Issue 3 https://doi.org/10.1107/S0108270189007948	journal	March 1990
Synthèse et structure du borouranate de calcium: CaB2U2O10 Gasperin, M. Acta Crystallographica Section C Crystal Structure Communications, Vol. 43, Issue 7 https://doi.org/10.1107/S0108270187092278	journal	July 1987
Synthèse et structure du tétraborouranate de nickel, Ni7B4UO16 Gasperin, M. Acta Crystallographica Section C Crystal Structure Communications, Vol. 45, Issue 7 https://doi.org/10.1107/S010827018900020X	journal	July 1989
Characterization of uranium borate (UB2O6) crystals Holcombe, C. E.; Johnson, D. H. Journal of Crystal Growth, Vol. 49, Issue 1 https://doi.org/10.1016/0022-0248(80)90085-8	journal	May 1980
Synthèse et structure du borouranate de sodium, NaBUO5 Gasperin, M. Acta Crystallographica Section C Crystal Structure Communications, Vol. 44, Issue 3 https://doi.org/10.1107/S0108270187011405	journal	March 1988
Structural Complexity of Barium Uranyl Arsenates: Synthesis, Structure, and Topology of Ba ₄ [(UO ₂ ) ₂ (As ₂ O ₇ ) ₃ ], Ba ₃ [(UO ₂ ) ₂ (AsO ₄ ) ₂ (As ₂ O ₇ )], and Ba ₅ Ca[(UO ₂ ) ₈ (AsO ₄ ) ₄ O ₈ ] Alekseev, Evgeny V.; Krivovichev, Sergey V.; Depmeier, Wulf Crystal Growth & Design, Vol. 11, Issue 7 https://doi.org/10.1021/cg200592s	journal	July 2011
Synthèse et structure du diborouranate de magnésium, MgB2UO7 Gasperin, M. Acta Crystallographica Section C Crystal Structure Communications, Vol. 43, Issue 12 https://doi.org/10.1107/S0108270187088139	journal	December 1987
Divergent Structural Chemistry of Uranyl Borates Obtained from Solid State and Hydrothermal Conditions Hao, Yucheng; Kegler, Philip; Bosbach, Dirk Crystal Growth & Design, Vol. 17, Issue 11 https://doi.org/10.1021/acs.cgd.7b00997	journal	October 2017
K2[(UO2)As2O7] – the First Uranium Polyarsenate Alekseev, Evgeny V.; Krivovichev, Sergey V.; Depmeier, Wulf Zeitschrift für anorganische und allgemeine Chemie, Vol. 633, Issue 8 https://doi.org/10.1002/zaac.200700020	journal	July 2007
How are Centrosymmetric and Noncentrosymmetric Structures Achieved in Uranyl Borates? Wang, Shuao; Alekseev, Evgeny V.; Stritzinger, Jared T. Inorganic Chemistry, Vol. 49, Issue 6 https://doi.org/10.1021/ic902480n	journal	March 2010
Uranium(VI) Adopts a Tetraoxido Core Wu, Shijun; Ling, Jie; Wang, Shuao European Journal of Inorganic Chemistry, Vol. 2009, Issue 27 https://doi.org/10.1002/ejic.200900658	journal	September 2009
Na2U2O7: Synthèse et structure d'un monocristal Gasperin, Madeleine Journal of the Less Common Metals, Vol. 119, Issue 1 https://doi.org/10.1016/0022-5088(86)90198-0	journal	May 1986
Cation–cation interaction in crystalline actinide compounds Krot, Nikolai N.; Grigoriev, Mikhail S. Russian Chemical Reviews, Vol. 73, Issue 1 https://doi.org/10.1070/RC2004v073n01ABEH000852	journal	January 2004
Cation-cation interactions between uranyl(VI) ions Serezhkin, V. N.; Sidorenko, G. V.; Pushkin, D. V. Radiochemistry, Vol. 56, Issue 2 https://doi.org/10.1134/S1066362214020015	journal	March 2014
CRYSTAL CHEMISTRY OF URANYL MOLYBDATES. VI. NEW URANYL MOLYBDATE UNITS IN THE STRUCTURES OF Cs4[(UO2)3O(MoO4)2(MoO5)] AND Cs6[(UO2)(MoO4)4] Krivovichev, S. V.; Burns, P. C. The Canadian Mineralogist, Vol. 40, Issue 1 https://doi.org/10.2113/gscanmin.40.1.201	journal	February 2002
CRYSTAL CHEMISTRY OF URANYL MOLYBDATES. III. NEW STRUCTURAL THEMES IN Na6[(UO2)2O(MoO4)4], Na6[(UO2)(MoO4)4] AND K6[(UO2)2O(MoO4)4] Krivovichev, S. V.; Burns, P. C. The Canadian Mineralogist, Vol. 39, Issue 1 https://doi.org/10.2113/gscanmin.39.1.197	journal	February 2001
Synthetic Strategies for the Synthesis of Ternary Uranium(IV) and Thorium(IV) Fluorides Klepov, Vladislav V.; Felder, Justin B.; zur Loye, Hans-Conrad Inorganic Chemistry, Vol. 57, Issue 9 https://doi.org/10.1021/acs.inorgchem.8b00570	journal	April 2018
Thermodynamic Assessment of P ₂ O ₅ Jung, In-Ho; Hudon, Pierre Journal of the American Ceramic Society, Vol. 95, Issue 11 https://doi.org/10.1111/j.1551-2916.2012.05382.x	journal	August 2012
Synthesis, Crystal Structure, and Comparison of Two New Uranyl Vanadate Layered Compounds: M6(UO2)5(VO4)2O5 with M=Na, K Dion, C.; Obbade, S.; Raekelboom, E. Journal of Solid State Chemistry, Vol. 155, Issue 2 https://doi.org/10.1006/jssc.2000.8923	journal	December 2000
Synthesis and crystal structure of α and β-Rb6U5V2O23, a new layered compound Obbade, S.; Dion, C.; Duvieubourg, L. Journal of Solid State Chemistry, Vol. 173, Issue 1 https://doi.org/10.1016/S0022-4596(03)00052-5	journal	June 2003
A novel open-framework with non-crossing channels in the uranyl vanadates A(UO2)4(VO4)3 (A=Li, Na) Obbade, S.; Dion, C.; Rivenet, M. Journal of Solid State Chemistry, Vol. 177, Issue 6 https://doi.org/10.1016/j.jssc.2004.02.011	journal	June 2004
Recent progress in actinide borate chemistry Wang, Shuao; Alekseev, Evgeny V.; Depmeier, Wulf Chemical Communications, Vol. 47, Issue 39 https://doi.org/10.1039/c1cc14023j	journal	January 2011
The Metal Flux: A Preparative Tool for the Exploration of Intermetallic Compounds Kanatzidis, Mercouri G.; Pöttgen, Rainer; Jeitschko, Wolfgang Angewandte Chemie International Edition, Vol. 44, Issue 43 https://doi.org/10.1002/anie.200462170	journal	November 2005
An Unprecedented Uranyl Phosphate Framework in the Structure of [(UO ₂ ) ₃ (PO ₄ )O(OH)(H ₂ O) ₂ ](H ₂ O) Burns, Peter C.; Alexopoulos, Cara M.; Hotchkiss, Peter J. Inorganic Chemistry, Vol. 43, Issue 6 https://doi.org/10.1021/ic0348547	journal	March 2004
Cation–cation interactions and cation exchange in a series of isostructural framework uranyl tungstates Balboni, Enrica; Burns, Peter C. Journal of Solid State Chemistry, Vol. 213 https://doi.org/10.1016/j.jssc.2014.02.001	journal	May 2014
Synthesis, structure, and spectroscopic characterization of three uranyl phosphates with unique structural units Wylie, Ernest M.; Dawes, Colleen M.; Burns, Peter C. Journal of Solid State Chemistry, Vol. 196 https://doi.org/10.1016/j.jssc.2012.07.020	journal	December 2012

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