A Telescoping View of Solute Architectures in a Complex Fluid System

Motokawa, Ryuhei; Kobayashi, Tohru; Endo, Hitoshi; Mu, Junju; Williams, Christopher D.; Masters, Andrew J.; Antonio, Mark R.; Heller, William T.; Nagao, Michihiro

doi:10.1021/acscentsci.8b00669

Title: A Telescoping View of Solute Architectures in a Complex Fluid System

Journal Article · 31 December 2018 · ACS Central Science

DOI: https://doi.org/10.1021/acscentsci.8b00669 · OSTI ID:1489165

^[1]; Kobayashi, Tohru ^[1]; Endo, Hitoshi ^[2];

^[3];

^[4];

^[5];

^[6]

Japan Atomic Energy Agency, Ibaraki (Japan)
Japan Atomic Energy Agency, Ibaraki (Japan); High Energy Accelerator Research Organization, Ibaraki (Japan); The Graduate Univ. of Advanced Studies (SOKENDAI), Ibaraki (Japan)
The Univ. of Manchester, Manchester (United Kingdom)
Argonne National Lab. (ANL), Lemont, IL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Indiana Univ., Bloomington, IN (United States)

Short- and long-range correlations between solutes in solvents can influence the macroscopic chemistry and physical properties of solutions in ways that are not fully understood. The class of liquids known as complex (structured) fluids—containing multiscale aggregates resulting from weak self-assembly—are especially important in energy-relevant systems employed for a variety of chemical- and biological-based purification, separation, and catalytic processes. In these, solute (mass) transfer across liquid-liquid (water, oil) phase boundaries is the core function. Oftentimes the operational success of phase transfer chemistry is dependent upon the bulk fluid structures for which a common functional motif and an archetype aggregate is the micelle. In particular, there is an emerging consensus that mass transfer and bulk organic phase behaviors—notably the critical phenomenon of phase splitting—are impacted by the effects of micellar-like aggregates in water-in-oil microemulsions. In this study, we elucidate the microscopic structures and mesoscopic architectures of metal-, water-, and acid-loaded organic phases using a combination of X-ray and neutron experimentation as well as density functional theory and molecular dynamics simulations. The key conclusion is that the transfer of metal ions between an aqueous phase and an organic one involves the formation of small mononuclear clusters typical of metal-ligand coordination chemistry, at one extreme, in the organic phase, and their aggregation to multinuclear primary clusters that self-assemble to form even larger super-clusters typical of supramolecular chemistry, at the other. Our metrical results add an orthogonal perspective to the energetics-based view of phase splitting in chemical separations known as the micellar model—founded upon the interpretation of small-angle neutron scattering data—with respect to a more general phase-space (gas-liquid) model of soft matter self-assembly and particle growth. Furthermore, the structure hierarchy observed in the aggregation of our quinary—zirconium nitrate–nitric acid–water–tri-n-butyl phosphate–n-octane—system is relevant to understanding solution phase transitions, in general, and the function of engineered fluids with metalloamphiphiles, in particular, for mass transfer applications, such as demixing in separation and synthesis in catalysis science.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1489165

Alternate ID(s):: OSTI ID: 1494559; OSTI ID: 1508830; OSTI ID: 1607238

Journal Information:: ACS Central Science, Vol. 5, Issue 1; ISSN 2374-7943

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 45 works

Citation information provided by
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Molecular Origins of Mesoscale Ordering in a Metalloamphiphile Phase Qiao, Baofu; Ferru, Geoffroy; Olvera de la Cruz, Monica ACS Central Science, Vol. 1, Issue 9 https://doi.org/10.1021/acscentsci.5b00306	journal	December 2015
Critical Exponents for Solvent Extraction Resolved Using SAXS Ellis, Ross J. The Journal of Physical Chemistry B, Vol. 118, Issue 1 https://doi.org/10.1021/jp408078v	journal	December 2013
Small‐Angle Neutron Scattering Study of Plutonium Third Phase Formation in 30% TBP/HNO ₃ /Alkane Diluent Systems Plaue, J.; Gelis, A.; Czerwinski, K. Solvent Extraction and Ion Exchange, Vol. 24, Issue 3 https://doi.org/10.1080/07366290600646970	journal	July 2006
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Monte Carlo calculations of cluster statistics in continuum models of composite morphology Sevick, E. M.; Monson, P. A.; Ottino, J. M. The Journal of Chemical Physics, Vol. 88, Issue 2 https://doi.org/10.1063/1.454720	journal	January 1988
Metal Recognition Driven by Weak Interactions: A Case Study in Solvent Extraction Poirot, Rémi; Le Goff, Xavier; Diat, Olivier ChemPhysChem, Vol. 17, Issue 14 https://doi.org/10.1002/cphc.201600305	journal	May 2016
Theoretical Modeling of Associated Structures in Aqueous Solutions of Hydrophobically Modified Telechelic PNIPAM Based on a Neutron Scattering Study Koga, Tsuyoshi; Tanaka, Fumihiko; Motokawa, Ryuhei Macromolecules, Vol. 41, Issue 23 https://doi.org/10.1021/ma800957z	journal	December 2008
Flexibility, persistence length and bicontinuous microstructures in microemulsions Zemb, Thomas Comptes Rendus Chimie, Vol. 12, Issue 1-2 https://doi.org/10.1016/j.crci.2008.10.008	journal	January 2009
Effect of n -Octanol on the Structure at the Supramolecular Scale of Concentrated Dimethyldioctylhexylethoxymalonamide Extractant Solutions Abécassis, B.; Testard, F.; Zemb, Th. Langmuir, Vol. 19, Issue 17 https://doi.org/10.1021/la034088g	journal	August 2003
Aggregation of Heteropolyanions in Aqueous Solutions Exhibiting Short-Range Attractions and Long-Range Repulsions Bera, Mrinal K.; Qiao, Baofu; Seifert, Soenke The Journal of Physical Chemistry C, Vol. 120, Issue 2 https://doi.org/10.1021/acs.jpcc.5b10609	journal	December 2015
Supramolecular solvents in the extraction of organic compounds. A review Ballesteros-Gómez, Ana; Sicilia, María Dolores; Rubio, Soledad Analytica Chimica Acta, Vol. 677, Issue 2 https://doi.org/10.1016/j.aca.2010.07.027	journal	September 2010
Third phase inversion, red oil formation, and multinuclear speciation of tetravalent cerium in the tri- n -butyl phosphate– n -dodecane solvent extraction system Antonio, Mark R.; Demars, Thomas J.; Audras, Matthieu Separation Science and Technology, Vol. 53, Issue 12 https://doi.org/10.1080/01496395.2017.1281303	journal	February 2017
Applications of Diglycolamide Based Solvent Extraction Processes in Spent Nuclear Fuel Reprocessing, Part 1: TODGA Whittaker, Daniel; Geist, Andreas; Modolo, Giuseppe Solvent Extraction and Ion Exchange, Vol. 36, Issue 3 https://doi.org/10.1080/07366299.2018.1464269	journal	April 2018
A neutron scattering study of the structure of a bimodal colloidal crystal Bartlett, P.; Ottewill, R. H. The Journal of Chemical Physics, Vol. 96, Issue 4 https://doi.org/10.1063/1.461926	journal	February 1992
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Catalytic Chemistry of Heteropoly Compounds Okuhara, Toshio; Mizuno, Noritaka; Misono, Makoto Advances in Catalysis https://doi.org/10.1016/S0360-0564(08)60041-3	book	January 1996

Cited By (2)

Extraction Performance of a Fluorous Phosphate for Zr(IV) from HNO ₃ Solution: Comparison with Tri- n -Butyl Phosphate Ueda, Yuki; Kikuchi, Kei; Sugita, Tsuyoshi Solvent Extraction and Ion Exchange, Vol. 37, Issue 5 https://doi.org/10.1080/07366299.2019.1638015	journal	July 2019
Amphiphile-Based Complex Fluids: The Self-Assembly Ensemble as Protagonist Clark, Aurora E. ACS Central Science, Vol. 5, Issue 1 https://doi.org/10.1021/acscentsci.8b00927	journal	December 2018

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
DFT
density functional theory
EXAFS
extended X-ray absorption fine structure
PUREX
Plutonium uranium reduction extraction
SANS
small-angle neutron scattering
Solvent extraction
Zirconium

Title: A Telescoping View of Solute Architectures in a Complex Fluid System

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