Two-Step Adsorption of PtCl 6 2– Complexes at a Charged Langmuir Monolayer: Role of Hydration and Ion Correlations

Uysal, Ahmet; Rock, William; Qiao, Baofu; Bu, Wei; Lin, Binhua

doi:10.1021/acs.jpcc.7b09350

Title: Two-Step Adsorption of PtCl ₆ ^2– Complexes at a Charged Langmuir Monolayer: Role of Hydration and Ion Correlations

Journal Article · Fri Nov 03 00:00:00 EDT 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b09350· OSTI ID:1408257

^[1]; Rock, William ^[1];

^[1];

^[2];

^[2]

Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
Center for Advanced Radiation Sources, The University of Chicago, Chicago, Illinois 60637, United States

Anion exchange at positively charged interfaces plays an important role in a variety of physical and chemical processes. However, the molecular-scale details of these processes, especially with heavy and large anionic complexes, are not well-understood. We studied the adsorption of PtCl62– anionic complexes to floating DPTAP monolayers in the presence of excess Cl– as a function of the bulk chlorometalate concentration. This system aims to simulate the industrial conditions for heavy metal separations with solvent extraction. In situ X-ray scattering and fluorescence measurements, which are element and depth sensitive, show that the chlorometalate ions only adsorb in the diffuse layer at lower concentrations, while they adsorb predominantly in the Stern layer at higher concentrations. The response of DPTAP molecules to the adsorbed ions is determined independently by grazing incidence X-ray diffraction and supports this picture. Molecular dynamics simulations further elucidate the nanoscale structure of the interfacial complexes. The results suggest that ion hydration and ion–ion correlations play a key role in the competitive adsorption process.

View Journal Article

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1408257

Alternate ID(s):: OSTI ID: 1421788; OSTI ID: 1426236; OSTI ID: 1507708

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Vol. 121 Journal Issue: 45; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 26 works

Citation information provided by
Web of Science

References (48)

Co-extraction of cations and anions in base metal recovery Tasker, Peter A.; Tong, Christine C.; Westra, Arjan N. Coordination Chemistry Reviews, Vol. 251, Issue 13-14 https://doi.org/10.1016/j.ccr.2007.03.014	journal	July 2007
Anion Receptor Design: Exploiting Outer-Sphere Coordination Chemistry To Obtain High Selectivity for Chloridometalates over Chloride Carson, Innis; MacRuary, Kirstian J.; Doidge, Euan D. Inorganic Chemistry, Vol. 54, Issue 17 https://doi.org/10.1021/acs.inorgchem.5b01317	journal	August 2015
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
Salt Promotes Protonation of Amine Groups at Air/Water Interface Sung, Woongmo; Avazbaeva, Zaure; Kim, Doseok The Journal of Physical Chemistry Letters, Vol. 8, Issue 15 https://doi.org/10.1021/acs.jpclett.7b01198	journal	July 2017
Tuning ion correlations at an electrified soft interface Laanait, N.; Mihaylov, M.; Hou, B. Proceedings of the National Academy of Sciences, Vol. 109, Issue 50 https://doi.org/10.1073/pnas.1214204109	journal	November 2012
Ion-Specific Induced Charges at Aqueous Soft Interfaces Wang, Wenjie; Park, Rebecca Y.; Travesset, Alex Physical Review Letters, Vol. 106, Issue 5 https://doi.org/10.1103/PhysRevLett.106.056102	journal	February 2011
Seven chemical separations to change the world Sholl, David S.; Lively, Ryan P. Nature, Vol. 532, Issue 7600 https://doi.org/10.1038/532435a	journal	April 2016
Specific Ion Effects at the Air/Water Interface Jungwirth, Pavel; Tobias, Douglas J. Chemical Reviews, Vol. 106, Issue 4 https://doi.org/10.1021/cr0403741	journal	April 2006
Solvent Extraction: Structure of the Liquid-Liquid Interface Containing a Diamide Ligand Scoppola, Ernesto; Watkins, Erik B.; Campbell, Richard A. Angewandte Chemie International Edition, Vol. 55, Issue 32 https://doi.org/10.1002/anie.201603395	journal	June 2016
Co-refinement of multiple-contrast neutron/X-ray reflectivity data using MOTOFIT Nelson, Andrew Journal of Applied Crystallography, Vol. 39, Issue 2 https://doi.org/10.1107/S0021889806005073	journal	March 2006
GROMACS 4: Algorithms for Highly Efficient, Load-Balanced, and Scalable Molecular Simulation Hess, Berk; Kutzner, Carsten; van der Spoel, David Journal of Chemical Theory and Computation, Vol. 4, Issue 3 https://doi.org/10.1021/ct700301q	journal	February 2008
Second harmonic generation monitoring of nitric acid extraction by a monoamide at the water–dodecane interface Martin-Gassin, G.; Gassin, P. M.; Couston, L. Physical Chemistry Chemical Physics, Vol. 13, Issue 43 https://doi.org/10.1039/c1cp22179e	journal	January 2011
Real-time observation of cation exchange kinetics and dynamics at the muscovite-water interface Lee, Sang Soo; Fenter, Paul; Nagy, Kathryn L. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15826	journal	June 2017
Observation of Ordered Structures in Counterion Layers near Wet Charged Surfaces: A Potential Mechanism for Charge Inversion Miller, Mitchell; Chu, Miaoqi; Lin, Binhua Langmuir, Vol. 32, Issue 1 https://doi.org/10.1021/acs.langmuir.5b04058	journal	December 2015
Liquid Surfaces and Interfaces: Synchrotron X-ray Methods Pershan, Peter S.; Schlossman, Mark https://doi.org/10.1017/CBO9781139045872	book	September 2012
Surface Studies of Solids by Total Reflection of X-Rays Parratt, L. G. Physical Review, Vol. 95, Issue 2 https://doi.org/10.1103/PhysRev.95.359	journal	July 1954
X-ray Reflectivity Reveals a Nonmonotonic Ion-Density Profile Perpendicular to the Surface of ErCl ₃ Aqueous Solutions Luo, Guangming; Bu, Wei; Mihaylov, Miroslav The Journal of Physical Chemistry C, Vol. 117, Issue 37 https://doi.org/10.1021/jp4067247	journal	September 2013
The Electrostatic Screening Length in Concentrated Electrolytes Increases with Concentration Smith, Alexander M.; Lee, Alpha A.; Perkin, Susan The Journal of Physical Chemistry Letters, Vol. 7, Issue 12 https://doi.org/10.1021/acs.jpclett.6b00867	journal	May 2016
Supramolecular Interactions in PuO ₂ Cl ₄ ^2– and PuCl ₆ ^2– Complexes with Protonated Pyridines: Synthesis, Crystal Structures, and Raman Spectroscopy Wilson, Richard E.; Schnaars, David D.; Andrews, Michael B. Inorganic Chemistry, Vol. 53, Issue 1 https://doi.org/10.1021/ic4023294	journal	December 2013
Structure and phase transitions in Langmuir monolayers Kaganer, Vladimir M.; Möhwald, Helmuth; Dutta, Pulak Reviews of Modern Physics, Vol. 71, Issue 3 https://doi.org/10.1103/RevModPhys.71.779	journal	April 1999
Erbium(III) Coordination at the Surface of an Aqueous Electrolyte Bera, Mrinal K.; Luo, Guangming; Schlossman, Mark L. The Journal of Physical Chemistry B, Vol. 119, Issue 28 https://doi.org/10.1021/acs.jpcb.5b02958	journal	May 2015
Investigations of the Hofmeister series and other specific ion effects using lipid model systems Leontidis, Epameinondas Advances in Colloid and Interface Science, Vol. 243 https://doi.org/10.1016/j.cis.2017.04.001	journal	May 2017
Polynuclear Speciation of Trivalent Cations near the Surface of an Electrolyte Solution Bera, Mrinal K.; Antonio, Mark R. Langmuir, Vol. 31, Issue 19 https://doi.org/10.1021/acs.langmuir.5b01354	journal	May 2015
Interfacial Water Structure Associated with Phospholipid Membranes Studied by Phase-Sensitive Vibrational Sum Frequency Generation Spectroscopy Chen, Xiangke; Hua, Wei; Huang, Zishuai Journal of the American Chemical Society, Vol. 132, Issue 32 https://doi.org/10.1021/ja1048237	journal	August 2010
Counterion Effect on Interfacial Water at Charged Interfaces and Its Relevance to the Hofmeister Series Nihonyanagi, Satoshi; Yamaguchi, Shoichi; Tahara, Tahei Journal of the American Chemical Society, Vol. 136, Issue 17 https://doi.org/10.1021/ja412952y	journal	April 2014
Quantity Separation of Rare Earths by Liquid—Liquid Extraction. I. The First Kilogram of Gadolinium Oxide ¹ Weaver, Boyd; Kappelmann, F. A.; Topp, A. C. Journal of the American Chemical Society, Vol. 75, Issue 16 https://doi.org/10.1021/ja01112a019	journal	August 1953
Electrical double layers at the oil/water interface Volkov, A. G.; Deamer, D. W.; Tanelian, D. L. Progress in Surface Science, Vol. 53, Issue 1 https://doi.org/10.1016/S0079-6816(97)82876-6	journal	September 1996
X-ray fluorescence spectroscopy from ions at charged vapor/water interfaces Bu, Wei; Vaknin, David Journal of Applied Physics, Vol. 105, Issue 8 https://doi.org/10.1063/1.3117487	journal	April 2009
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
Preparation of colloidal gold by photoreduction of tetracyanoaurate(1-)-cationic surfactant complexes Torigoe, Kanjiro; Esumi, Kunio Langmuir, Vol. 8, Issue 1 https://doi.org/10.1021/la00037a013	journal	January 1992
Electrostatic correlations: from plasma to biology Levin, Yan Reports on Progress in Physics, Vol. 65, Issue 11 https://doi.org/10.1088/0034-4885/65/11/201	journal	September 2002
Atomic Number Dependent “Structural Transitions” in Ordered Lanthanide Monolayers: Role of the Hydration Shell Miller, Mitchell; Chu, Miaoqi; Lin, Binhua Langmuir, Vol. 33, Issue 6 https://doi.org/10.1021/acs.langmuir.6b04609	journal	January 2017
Reverse Self-Assembly: (111)-Oriented Gold Crystallization at Alkylthiol Monolayer Templates Uysal, Ahmet; Stripe, Benjamin; Lin, Binhua Physical Review Letters, Vol. 107, Issue 11 https://doi.org/10.1103/PhysRevLett.107.115503	journal	September 2011
Optimization of the Additive CHARMM All-Atom Protein Force Field Targeting Improved Sampling of the Backbone ϕ, ψ and Side-Chain χ ₁ and χ ₂ Dihedral Angles Best, Robert B.; Zhu, Xiao; Shim, Jihyun Journal of Chemical Theory and Computation, Vol. 8, Issue 9 https://doi.org/10.1021/ct300400x	journal	August 2012
Molecular Scale Description of Anion Competition on Amine-Functionalized Surfaces Rock, William; Oruc, Muhammed E.; Ellis, Ross J. Langmuir, Vol. 32, Issue 44 https://doi.org/10.1021/acs.langmuir.6b03479	journal	October 2016
Estimation of the Thermochemical Radii and Ionic Volumes of Complex Ions Simoes, Marcus C.; Hughes, Kevin J.; Ingham, Derek B. Inorganic Chemistry, Vol. 56, Issue 13 https://doi.org/10.1021/acs.inorgchem.7b01205	journal	June 2017
Specific Anion Effects on Water Structure Adjacent to Protein Monolayers ^† Chen, Xin; Flores, Sarah C.; Lim, Soon-Mi Langmuir, Vol. 26, Issue 21 https://doi.org/10.1021/la1015862	journal	November 2010
Modeling Platinum Group Metal Complexes in Aqueous Solution Lienke, Achim; Klatt, Günter; Robinson, David J. Inorganic Chemistry, Vol. 40, Issue 10 https://doi.org/10.1021/ic0005745	journal	May 2001
Beyond Hofmeister Jungwirth, Pavel; Cremer, Paul S. Nature Chemistry, Vol. 6, Issue 4 https://doi.org/10.1038/nchem.1899	journal	March 2014
Solvent extraction of platinum using amine based extractants in different solutions: A review Jha, Manis Kumar; Gupta, Divika; Lee, Jae-chun Hydrometallurgy, Vol. 142 https://doi.org/10.1016/j.hydromet.2013.11.009	journal	February 2014
The liquid surface/interface spectrometer at ChemMatCARS synchrotron facility at the Advanced Photon Source Lin, Binhua; Meron, Mati; Gebhardt, Jeff Physica B: Condensed Matter, Vol. 336, Issue 1-2 https://doi.org/10.1016/S0921-4526(03)00272-2	journal	August 2003
From Franklin to Today: Toward a Molecular Level Understanding of Bonding and Adsorption at the Oil−Water Interface McFearin, Cathryn L.; Beaman, Daniel K.; Moore, Fred G. The Journal of Physical Chemistry C, Vol. 113, Issue 4 https://doi.org/10.1021/jp808212m	journal	December 2008
Investigation of Structure, Adsorption Free Energy, and Overcharging Behavior of Trivalent Yttrium Adsorbed at the Muscovite (001)–Water Interface Lee, Sang Soo; Schmidt, Moritz; Laanait, Nouamane The Journal of Physical Chemistry C, Vol. 117, Issue 45 https://doi.org/10.1021/jp407693x	journal	October 2013
Specificity and Variation of Length Scale over Which Monovalent Halide Ions Neutralize a Charged Interface Sung, Woongmo; Wang, Wenjie; Lee, Jonggwan The Journal of Physical Chemistry C, Vol. 119, Issue 13 https://doi.org/10.1021/jp512233g	journal	March 2015
A Simple Primary Amide for the Selective Recovery of Gold from Secondary Resources Doidge, Euan D.; Carson, Innis; Tasker, Peter A. Angewandte Chemie International Edition, Vol. 55, Issue 40 https://doi.org/10.1002/anie.201606113	journal	August 2016
A simple empirical model describing the thermodynamics of hydration of ions of widely varying charges, sizes, and shapes Marcus, Yizhak Biophysical Chemistry, Vol. 51, Issue 2-3 https://doi.org/10.1016/0301-4622(94)00051-4	journal	August 1994
How Accurate Is Poisson−Boltzmann Theory for Monovalent Ions near Highly Charged Interfaces? Bu, Wei; Vaknin, David; Travesset, Alex Langmuir, Vol. 22, Issue 13 https://doi.org/10.1021/la053400e	journal	June 2006
Implementation of the CHARMM Force Field in GROMACS: Analysis of Protein Stability Effects from Correction Maps, Virtual Interaction Sites, and Water Models Bjelkmar, Pär; Larsson, Per; Cuendet, Michel A. Journal of Chemical Theory and Computation, Vol. 6, Issue 2 https://doi.org/10.1021/ct900549r	journal	January 2010

Similar Records

Chemical Potential Driven Reorganization of Anions between Stern and Diffuse Layers at the Air/Water Interface

Journal Article · Thu Jan 06 00:00:00 EST 2022 · Journal of Physical Chemistry. C · OSTI ID:1408257

Kumal, Raju R.; Nayak, Srikanth; Bu, Wei; +1 more

Heavy Anionic Complex Creates a Unique Water Structure at a Soft Charged Interface

Journal Article · Mon Nov 19 00:00:00 EST 2018 · Journal of Physical Chemistry. C · OSTI ID:1408257

Rock, William; Qiao, Baofu; Zhou, Tiecheng; +2 more

Zn2+ and Sr2+ Adsorption at the TiO2 (110)-Electrolyte Interface: Influence of Ionic Strength, Coverage, and Anions

Journal Article · Sun Jan 01 00:00:00 EST 2006 · J. Colloid Interface Sci. · OSTI ID:1408257

Zhang, Z; Fenter, P; Cheng, L; +5 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Two-Step Adsorption of PtCl 6 2– Complexes at a Charged Langmuir Monolayer: Role of Hydration and Ion Correlations

Citation Formats

References (48)

Similar Records

Related Subjects

Title: Two-Step Adsorption of PtCl ₆ ^2– Complexes at a Charged Langmuir Monolayer: Role of Hydration and Ion Correlations