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Title: Origins of Clustering of Metalate–Extractant Complexes in Liquid–Liquid Extraction

Abstract

Effective and energy-efficient separation of precious and rare metals is very important for a variety of advanced technologies. Liquid-liquid extraction (LLE) is a relatively less energy intensive separation technique, widely used in separation of lanthanides, actinides, and platinum group metals (PGMs). In LLE, the distribution of an ion between an aqueous phase and an organic phase is determined by enthalpic (coordination interactions) and entropic (fluid reorganization) contributions. The molecular scale details of these contributions are not well understood. Preferential extraction of an ion from the aqueous phase is usually correlated with the resulting fluid organization in the organic phase, as the longer-range organization increases with metal loading. However, it is difficult to determine the extent to which organic phase fluid organization causes, or is caused by, metal loading. In this study, we demonstrate that two systems with the same metal loading may impart very different organic phase organizations and investigate the underlying molecular scale mechanism. Small-angle X-ray scattering shows that the structure of a quaternary ammonium extractant solution in toluene is affected differently by the extraction of two metalates (octahedral PtCl62- and square-planar PtCl62-), although both are completely transferred into the organic phase. The aggregates formed by the metalate-extractant complexesmore » (approximated as reverse micelles) exhibit a more long-range order (clustering) with PtCl62- compared to that with PtCl62-. Vibrational sum frequency generation spectroscopy and complementary atomistic molecular dynamics simulations on model Langmuir monolayers indicate that the two metalates affect the interfacial hydration structures differently. Furthermore, the interfacial hydration is correlated with water extraction into the organic phase. Overall, these results support a strong relationship between the organic phase organizational structure and the different local hydration present within the aggregates of metalate-extractant complexes, which is independent of metalate concentration.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
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  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Washington State Univ., Pullman, WA (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); National Aeronautics and Space Administration (NASA)
OSTI Identifier:
1845340
Grant/Contract Number:  
AC02-06CH11357; SC0001815; CHE-1834750; NNA04CC36G
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 13; Journal Issue: 20; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; liquid-liquid extraction; small-angle X-ray scattering; complex fluids; amphiphile aggregation; vibrational sum frequency generation; ion hydration; interfaces; metals; liquid liquid equilibrium; chemical structure; extraction

Citation Formats

Nayak, Srikanth, Kumal, Raju R., Liu, Zhu, Qiao, Baofu, Clark, Aurora E., and Uysal, Ahmet. Origins of Clustering of Metalate–Extractant Complexes in Liquid–Liquid Extraction. United States: N. p., 2021. Web. doi:10.1021/acsami.0c23158.
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Nayak, Srikanth, Kumal, Raju R., Liu, Zhu, Qiao, Baofu, Clark, Aurora E., & Uysal, Ahmet. Origins of Clustering of Metalate–Extractant Complexes in Liquid–Liquid Extraction. United States. https://doi.org/10.1021/acsami.0c23158
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Nayak, Srikanth, Kumal, Raju R., Liu, Zhu, Qiao, Baofu, Clark, Aurora E., and Uysal, Ahmet. Tue . "Origins of Clustering of Metalate–Extractant Complexes in Liquid–Liquid Extraction". United States. https://doi.org/10.1021/acsami.0c23158. https://www.osti.gov/servlets/purl/1845340.
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@article{osti_1845340,
title = {Origins of Clustering of Metalate–Extractant Complexes in Liquid–Liquid Extraction},
author = {Nayak, Srikanth and Kumal, Raju R. and Liu, Zhu and Qiao, Baofu and Clark, Aurora E. and Uysal, Ahmet},
abstractNote = {Effective and energy-efficient separation of precious and rare metals is very important for a variety of advanced technologies. Liquid-liquid extraction (LLE) is a relatively less energy intensive separation technique, widely used in separation of lanthanides, actinides, and platinum group metals (PGMs). In LLE, the distribution of an ion between an aqueous phase and an organic phase is determined by enthalpic (coordination interactions) and entropic (fluid reorganization) contributions. The molecular scale details of these contributions are not well understood. Preferential extraction of an ion from the aqueous phase is usually correlated with the resulting fluid organization in the organic phase, as the longer-range organization increases with metal loading. However, it is difficult to determine the extent to which organic phase fluid organization causes, or is caused by, metal loading. In this study, we demonstrate that two systems with the same metal loading may impart very different organic phase organizations and investigate the underlying molecular scale mechanism. Small-angle X-ray scattering shows that the structure of a quaternary ammonium extractant solution in toluene is affected differently by the extraction of two metalates (octahedral PtCl62- and square-planar PtCl62-), although both are completely transferred into the organic phase. The aggregates formed by the metalate-extractant complexes (approximated as reverse micelles) exhibit a more long-range order (clustering) with PtCl62- compared to that with PtCl62-. Vibrational sum frequency generation spectroscopy and complementary atomistic molecular dynamics simulations on model Langmuir monolayers indicate that the two metalates affect the interfacial hydration structures differently. Furthermore, the interfacial hydration is correlated with water extraction into the organic phase. Overall, these results support a strong relationship between the organic phase organizational structure and the different local hydration present within the aggregates of metalate-extractant complexes, which is independent of metalate concentration.},
doi = {10.1021/acsami.0c23158},
journal = {ACS Applied Materials and Interfaces},
number = 20,
volume = 13,
place = {United States},
year = {Tue Apr 13 00:00:00 EDT 2021},
month = {Tue Apr 13 00:00:00 EDT 2021}
}
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