Predicting the Solubility of Inorganic Ion Pairs in Water

Rahman, Tasnim; Petrus, Enric; Segado, Mireia; Martin, Nicolas P.; Palys, Lauren N.; Rambaran, Mark A.; Ohlin, C. Andre; Bo, Carles; Nyman, May

doi:10.1002/anie.202117839

Title: Predicting the Solubility of Inorganic Ion Pairs in Water

Journal Article · 11 February 2022 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202117839 · OSTI ID:1976280

Rahman, Tasnim ^[1]; Petrus, Enric ^[2]; Segado, Mireia ^[2]; Martin, Nicolas P. ^[1]; Palys, Lauren N. ^[1]; Rambaran, Mark A. ^[3]; Ohlin, C. Andre ^[3]; Bo, Carles ^[4];

^[1]

Oregon State University, Corvallis, OR (United States)
Barcelona Institute of Science & Technology (BIST), Tarragona (Spain)
Umea University (Sweden)
Barcelona Institute of Science & Technology (BIST), Tarragona (Spain); Universitat Rovira i Virgili (URV), Tarragona (Spain)

Abstract Polyoxometalates (POMs), ranging in size from 1 to 10’s of nanometers, resemble building blocks of inorganic materials. Elucidating their complex solubility behavior with alkali‐counterions can inform natural and synthetic aqueous processes. In the study of POMs ([Nb ₂₄ O ₇₂ H ₉ ] ¹⁵⁻ , Nb ₂₄ ) we discovered an unusual solubility trend (termed anomalous solubility) of alkali‐POMs, in which Nb ₂₄ is most soluble with the smallest (Li ⁺ ) and largest (Rb/Cs ⁺ ) alkalis, and least soluble with Na/K ⁺ . Via computation, we define a descriptor (σ‐profile) and use an artificial neural network (ANN) to predict all three described alkali‐anion solubility trends: amphoteric, normal (Li ⁺ >Na ⁺ >K ⁺ >Rb ⁺ >Cs ⁺ ), and anomalous (Cs ⁺ >Rb ⁺ >K ⁺ >Na ⁺ >Li ⁺ ). Testing predicted amphoteric solubility affirmed the accuracy of the descriptor, provided solution‐phase snapshots of alkali–POM interactions, yielded a new POM formulated [Ti ₆ Nb ₁₄ O ₅₄ ] ¹⁴⁻ , and provides guidelines to exploit alkali–POM interactions for new POMs discovery.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Oregon State Univ., Corvallis, OR (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); Spanish Ministry of Science and Innovation; Severo Ochoa Excellence Accreditation; Catalan Institute of Chemical Research (ICIQ); Murdock Charitable Trust; Swedish Research Council (SRC); Kempe Foundation; USDOE

Grant/Contract Number:: SC0010802; PID2020-112806RB-I00; CEX2019-000925-S, MCI/AEI; SR-2017297; 2018-07039; JCK-2029.1

OSTI ID:: 1976280

Alternate ID(s):: OSTI ID: 1846505

Journal Information:: Angewandte Chemie (International Edition), Vol. 61, Issue 19; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (54)

Reaction Dynamics of the Decaniobate Ion [HxNb10O28](6−x)− in Water Villa, Eric M.; Ohlin, C. André; Balogh, Edina Angewandte Chemie, Vol. 120, Issue 26 https://doi.org/10.1002/ange.200801125	journal	June 2008
Sigma Profile Database for Predicting Solid Solubility in Pure and Mixed Solvent Mixtures for Organic Pharmacological Compounds with COSMO-Based Thermodynamic Methods Mullins, Eric; Liu, Y. A.; Ghaderi, Adel Industrial & Engineering Chemistry Research, Vol. 47, Issue 5 https://doi.org/10.1021/ie0711022	journal	March 2008
Giant Polyniobate Clusters Based on [Nb7O22]9− Units Derived from a Nb6O19 Precursor Niu, Jingyang; Ma, Pengtao; Niu, Hongyu Chemistry - A European Journal, Vol. 13, Issue 31 https://doi.org/10.1002/chem.200700612	journal	October 2007
Soluble Heteropolyniobates from the Bottom of Group IA Hou, Yu; Nyman, May; Rodriguez, Mark A. Angewandte Chemie, Vol. 123, Issue 52 https://doi.org/10.1002/ange.201104478	journal	September 2011
Crystallization by particle attachment in synthetic, biogenic, and geologic environments De Yoreo, J. J.; Gilbert, P. U. P. A.; Sommerdijk, N. A. J. M. Science, Vol. 349, Issue 6247 https://doi.org/10.1126/science.aaa6760	journal	July 2015
Evolution of Polyoxoniobate Cluster Anions Bontchev, Ranko P.; Nyman, May Angewandte Chemie, Vol. 118, Issue 40 https://doi.org/10.1002/ange.200602200	journal	October 2006
Metal ions and RNA folding: a highly charged topic with a dynamic future Woodson, Sarah A. Current Opinion in Chemical Biology, Vol. 9, Issue 2 https://doi.org/10.1016/j.cbpa.2005.02.004	journal	April 2005
Microwave Synthesis of Alkali‐Free Hexaniobate, Decaniobate, and Hexatantalate Polyoxometalate Ions Rambaran, Mark A.; Pascual‐Borràs, Magda; Ohlin, C. André European Journal of Inorganic Chemistry, Vol. 2019, Issue 35 https://doi.org/10.1002/ejic.201900750	journal	September 2019
Synthesis, structure, and molecular modeling of a titanoniobate isopolyanion Nyman, May; Criscenti, Louise J.; Bonhomme, François Journal of Solid State Chemistry, Vol. 176, Issue 1 https://doi.org/10.1016/S0022-4596(03)00354-2	journal	November 2003
Self-Assembly of Short Chain Poly- N -isopropylacrylamid Induced by Superchaotropic Keggin Polyoxometalates: From Globules to Sheets Buchecker, Thomas; Schmid, Philipp; Grillo, Isabelle Journal of the American Chemical Society, Vol. 141, Issue 17 https://doi.org/10.1021/jacs.8b12181	journal	April 2019
Beyond Charge Balance: Counter‐Cations in Polyoxometalate Chemistry Misra, Archismita; Kozma, Karoly; Streb, Carsten Angewandte Chemie International Edition, Vol. 59, Issue 2 https://doi.org/10.1002/anie.201905600	journal	January 2020
Reaction Dynamics of the Decaniobate Ion [HxNb10O28](6−x)− in Water Villa, Eric M.; Ohlin, C. André; Balogh, Edina Angewandte Chemie International Edition, Vol. 47, Issue 26 https://doi.org/10.1002/anie.200801125	journal	June 2008
Polyoxoniobates as molecular building blocks in thin films Rambaran, Mark A.; Gorzsás, András; Holmboe, Michael Dalton Transactions, Vol. 50, Issue 44 https://doi.org/10.1039/D1DT03116C	journal	January 2021
Self-Assembly and Phase Behavior of Germanium Oxide Nanoparticles in Basic Aqueous Solutions Rimer, Jeffrey D.; Roth, Daniel D.; Vlachos, Dionisios G. Langmuir, Vol. 23, Issue 5 https://doi.org/10.1021/la062828q	journal	February 2007
Der chaotrope Effekt als Aufbaumotiv in der Chemie Assaf, Khaleel I.; Nau, Werner M. Angewandte Chemie, Vol. 130, Issue 43 https://doi.org/10.1002/ange.201804597	journal	September 2018
Cesium salts of niobo-tungstate isopolyanions with intermediate group V–group VI character Sures, Dylan J.; Molina, Pedro I.; Miró, Pere New Journal of Chemistry, Vol. 40, Issue 2 https://doi.org/10.1039/C5NJ02914G	journal	January 2016
Models and mechanisms of Hofmeister effects in electrolyte solutions, and colloid and protein systems revisited Salis, Andrea; Ninham, Barry W. Chem. Soc. Rev., Vol. 43, Issue 21 https://doi.org/10.1039/C4CS00144C	journal	January 2014
Deliberate Construction of Polyoxoniobates Exploiting the Carbonate Ligand Amiri, Mehran; Martin, Nicolas P.; Feng, Ching‐Lei Angewandte Chemie International Edition, Vol. 60, Issue 22 https://doi.org/10.1002/anie.202017367	journal	April 2021
Machine learning with physicochemical relationships: solubility prediction in organic solvents and water Boobier, Samuel; Hose, David R. J.; Blacker, A. John Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-19594-z	journal	November 2020
Salt Effects on Protein Folding Thermodynamics Maity, Hiranmay; Muttathukattil, Aswathy N.; Reddy, Govardhan The Journal of Physical Chemistry Letters, Vol. 9, Issue 17 https://doi.org/10.1021/acs.jpclett.8b02220	journal	August 2018
Deliberate Construction of Polyoxoniobates Exploiting the Carbonate Ligand Amiri, Mehran; Martin, Nicolas P.; Feng, Ching‐Lei Angewandte Chemie, Vol. 133, Issue 22 https://doi.org/10.1002/ange.202017367	journal	April 2021
Soluble Heteropolyniobates from the Bottom of Group IA Hou, Yu; Nyman, May; Rodriguez, Mark A. Angewandte Chemie International Edition, Vol. 50, Issue 52 https://doi.org/10.1002/anie.201104478	journal	September 2011
Alkali-Driven Disassembly and Reassembly of Molecular Niobium Oxide in Water Sures, Dylan; Segado, Mireia; Bo, Carles Journal of the American Chemical Society, Vol. 140, Issue 34 https://doi.org/10.1021/jacs.8b05015	journal	July 2018
A new titanoniobate ion—completing the series [Nb10O28]6−, [TiNb9O28]7− and [Ti2Nb8O28]8− Ohlin, C. André; Villa, Eric M.; Fettinger, James C. Dalton Transactions, Issue 15 https://doi.org/10.1039/b900465c	journal	January 2009
Water-Mediated Ion Pairing: Occurrence and Relevance van der Vegt, Nico F. A.; Haldrup, Kristoffer; Roke, Sylvie Chemical Reviews, Vol. 116, Issue 13 https://doi.org/10.1021/acs.chemrev.5b00742	journal	April 2016
Structure–Activity Relationships for the Affinity of Chaotropic Polyoxometalate Anions towards Proteins Solé‐Daura, Albert; Poblet, Josep M.; Carbó, Jorge J. Chemistry – A European Journal, Vol. 26, Issue 26 https://doi.org/10.1002/chem.201905533	journal	April 2020
Anionic and Cationic Hofmeister Effects on Hydrophobic and Hydrophilic Surfaces Schwierz, Nadine; Horinek, Dominik; Netz, Roland R. Langmuir, Vol. 29, Issue 8 https://doi.org/10.1021/la303924e	journal	February 2013
Beyond the Hofmeister Series: Ion-Specific Effects on Proteins and Their Biological Functions Okur, Halil I.; Hladílková, Jana; Rembert, Kelvin B. The Journal of Physical Chemistry B, Vol. 121, Issue 9 https://doi.org/10.1021/acs.jpcb.6b10797	journal	February 2017
Solvent-shared pairs of densely charged ions induce intense but short-range supra-additive slowdown of water rotation Vila Verde, Ana; Santer, Mark; Lipowsky, Reinhard Physical Chemistry Chemical Physics, Vol. 18, Issue 3 https://doi.org/10.1039/C5CP05726D	journal	January 2016
A comprehensive comparison of transition-metal and actinyl polyoxometalates Nyman, May; Burns, Peter C. Chemical Society Reviews, Vol. 41, Issue 22 https://doi.org/10.1039/c2cs35136f	journal	January 2012
Directional Bonding in Decaniobate Inorganic Frameworks Martin, Nicolas P.; Nyman, May Angewandte Chemie, Vol. 133, Issue 2 https://doi.org/10.1002/ange.202010902	journal	November 2020
Pushing the limits of solubility prediction via quality-oriented data selection Sorkun, Murat Cihan; Koelman, J. M. Vianney A.; Er, Süleyman iScience, Vol. 24, Issue 1 https://doi.org/10.1016/j.isci.2020.101961	journal	January 2021
Polyoxoniobate chemistry in the 21st century Nyman, May Dalton Transactions, Vol. 40, Issue 32 https://doi.org/10.1039/c1dt10435g	journal	January 2011
Conductor-like Screening Model for Real Solvents: A New Approach to the Quantitative Calculation of Solvation Phenomena Klamt, Andreas The Journal of Physical Chemistry, Vol. 99, Issue 7 https://doi.org/10.1021/j100007a062	journal	February 1995
Co-ion Effects in the Self-Assembly of Macroions: From Co-ions to Co-macroions and to the Unique Feature of Self-Recognition Chen, Jiahui; Qian, Kun; Xiao, Kexing Langmuir, Vol. 36, Issue 35 https://doi.org/10.1021/acs.langmuir.0c01797	journal	August 2020
Jenseits von Ladungsausgleich: Gegenkationen in der Polyoxometallat‐Chemie Misra, Archismita; Kozma, Karoly; Streb, Carsten Angewandte Chemie, Vol. 132, Issue 2 https://doi.org/10.1002/ange.201905600	journal	October 2019
The atomic level journey from aqueous polyoxometalate to metal oxide Hou, Yu; Fast, Dylan B.; Ruther, Rose E. Journal of Solid State Chemistry, Vol. 221 https://doi.org/10.1016/j.jssc.2014.09.039	journal	January 2015
Oxygen-Isotope Exchange Rates for Three Isostructural Polyoxometalate Ions Villa, Eric M.; Ohlin, C. André; Casey, William H. Journal of the American Chemical Society, Vol. 132, Issue 14 https://doi.org/10.1021/ja100490n	journal	April 2010
Icosaniobate: A New Member of the Isoniobate Family Maekawa, Masaki; Ozawa, Yoshiki; Yagasaki, Atsushi Inorganic Chemistry, Vol. 45, Issue 24 https://doi.org/10.1021/ic0601788	journal	November 2006
Stable Prenucleation Calcium Carbonate Clusters Gebauer, Denis; Völkel, Antje; Cölfen, Helmut Science, Vol. 322, Issue 5909 https://doi.org/10.1126/science.1164271	journal	December 2008
Beyond Hofmeister Jungwirth, Pavel; Cremer, Paul S. Nature Chemistry, Vol. 6, Issue 4 https://doi.org/10.1038/nchem.1899	journal	March 2014
Lithium Polyniobates. A Lindqvist-Supported Lithium−Water Adamantane Cluster and Conversion of Hexaniobate to a Discrete Keggin Complex Anderson, Travis M.; Thoma, Steven G.; Bonhomme, François Crystal Growth & Design, Vol. 7, Issue 4 https://doi.org/10.1021/cg0606904	journal	April 2007
Directional Bonding in Decaniobate Inorganic Frameworks Martin, Nicolas P.; Nyman, May Angewandte Chemie International Edition, Vol. 60, Issue 2 https://doi.org/10.1002/anie.202010902	journal	November 2020
Strategic Capture of the {Nb ₇ } Polyoxometalate Martin, Nicolas P.; Petrus, Enric; Segado, Mireia Chemistry – A European Journal, Vol. 25, Issue 45 https://doi.org/10.1002/chem.201902770	journal	July 2019
The effect of calcium on aqueous uranium(VI) speciation and adsorption to ferrihydrite and quartz Fox, Patricia M.; Davis, James A.; Zachara, John M. Geochimica et Cosmochimica Acta, Vol. 70, Issue 6 https://doi.org/10.1016/j.gca.2005.11.027	journal	March 2006
Evolution of Polyoxoniobate Cluster Anions Bontchev, Ranko P.; Nyman, May Angewandte Chemie International Edition, Vol. 45, Issue 40 https://doi.org/10.1002/anie.200602200	journal	October 2006
Expanding the Schulze-Hardy Rule and the Hofmeister Series to Nanometer-Scaled Hydrophilic Macroions Chu, Yang; Chen, Jiahui; Haso, Fadi Chemistry - A European Journal, Vol. 24, Issue 21 https://doi.org/10.1002/chem.201706101	journal	March 2018
Influence of Ion Solvation on the Properties of Electrolyte Solutions Andreev, Marat; de Pablo, Juan J.; Chremos, Alexandros The Journal of Physical Chemistry B, Vol. 122, Issue 14 https://doi.org/10.1021/acs.jpcb.8b00518	journal	April 2018
The Chaotropic Effect as an Assembly Motif in Chemistry Assaf, Khaleel I.; Nau, Werner M. Angewandte Chemie International Edition, Vol. 57, Issue 43 https://doi.org/10.1002/anie.201804597	journal	September 2018
High-Throughput, In Silico Prediction of Aqueous Solubility Based on One- and Two-Dimensional Descriptors Engkvist, Ola; Wrede, Paul Journal of Chemical Information and Computer Sciences, Vol. 42, Issue 5 https://doi.org/10.1021/ci0202685	journal	August 2002
Octahedral clusters with mixed inner ligand environment: Self-assembly, modification and isomerism Naumov, N. G.; Brylev, K. A.; Mironov, Y. V. Journal of Structural Chemistry, Vol. 55, Issue 8 https://doi.org/10.1134/S0022476614080010	journal	December 2014
Can Polyoxometalates Be Considered as Superchaotropic Ions? Drummond, Carlos; Pérez-Fuentes, Leonor; Bastos-González, Delfi The Journal of Physical Chemistry C, Vol. 123, Issue 47 https://doi.org/10.1021/acs.jpcc.9b08324	journal	November 2019
Nanoparticulate Iron Oxide Minerals in Soils and Sediments: Unique Properties and Contaminant Scavenging Mechanisms Waychunas, Glenn A.; Kim, Christopher S.; Banfield, Jillian F. Journal of Nanoparticle Research, Vol. 7, Issue 4-5 https://doi.org/10.1007/s11051-005-6931-x	journal	October 2005
Redox properties of polyoxometalates: new insights on the anion charge effect López, Xavier; Fernández, Jorge A.; Poblet, Josep M. Dalton Trans., Issue 9 https://doi.org/10.1039/B507599H	journal	January 2006

Linked Research (6)

Figures / Tables (5)

Similar Records

Predicting the Solubility of Inorganic Ion Pairs in Water

Journal Article · 2022 · Angewandte Chemie · OSTI ID:1846492

Rahman, Tasnim; Petrus, Enric; Segado, Mireia; +6 more

Directional Bonding in Decaniobate Inorganic Frameworks

Journal Article · 2020 · Angewandte Chemie · OSTI ID:1786027

Martin, Nicolas P.; Nyman, May

Directional Bonding in Decaniobate Inorganic Frameworks

Journal Article · 2020 · Angewandte Chemie (International Edition) · OSTI ID:1786204