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Title: La3+ and Y3+ interactions with the carboxylic acid moiety at the liquid/vapor interface: Identification of binding complexes, charge reversal, and detection limits

Abstract

Specific interactions of yttrium and lanthanum ions with a fatty acid Langmuir monolayer were investigated using vibrational sum frequency spectroscopy. The trivalent ions were shown to interact with the charged form of the carboxylic acid group from nanomolar concentrations (<300 nM). Analysis of the spectral features from both the symmetric and the asymmetric carboxylate modes reveals the presence of at least three distinct coordination structures linked to specific binding configurations. Although the same species were identified for both La3+ and Y3+, they display a different concentration dependence, highlighting the ion-specificity of the interaction. From the analysis of the response of interfacial water molecules, the reversal of the surface charge, as well as the formation of yttrium hydroxide complexes, were detected upon increasing the amount of salt in solution. The binding interaction and kinetics of absorption are sensitive to the solution pH, showing a distinct ion speciation in the interfacial region when compared to the bulk. Changing the subphase pH or adding a monovalent background electrolyte that promotes deprotonation of the carboxylic acid headgroup could further improve the detection limit of La3+ and Y3+ to concentrations < 100 nM. These findings demonstrate that nM concentrations of trace metals contaminants, typically foundmore » on monovalent salts, can significantly influence the binding structure and kinetics in Langmuir monolayers.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [1]
+ Show Author Affiliations
  1. KTH Royal Inst. of Technology, Stockholm (Sweden)
  2. The Ohio State Univ., Columbus, OH (United States); Ruhr-Univ. Bochum (Germany)
  3. KTH Royal Inst. of Technology, Stockholm (Sweden); AMOLF, Amsterdam (The Netherlands)
  4. KTH Royal Inst. of Technology, Stockholm (Sweden); Australian National Univ., Canberra, ACT (Australia)
  5. The Ohio State Univ., Columbus, OH (United States)
Publication Date:
Research Org.:
The Ohio State Univ., Columbus, OH (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1830737
Grant/Contract Number:  
SC0022099
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Colloid and Interface Science
Additional Journal Information:
Journal Volume: 608; Journal Issue: Part 2; Journal ID: ISSN 0021-9797
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES; 04 OIL SHALES AND TAR SANDS; 01 COAL, LIGNITE, AND PEAT; Ion specific effects; Langmuir monolayer; Trivalent ions; Carboxylic acid moiety; Vibrational sum frequency spectroscopy; Molecular characterization; Carboxylate binding complexes; Charge reversal; Poisson Boltzmann theory; Vibrational spectroscopy; Arachidic acid; Eicosanoic acid monolayer

Citation Formats

Sthoer, Adrien, Adams, Ellen M., Sengupta, Sanghamitra, Corkery, Robert W., Allen, Heather C., and Tyrode, Eric C. La3+ and Y3+ interactions with the carboxylic acid moiety at the liquid/vapor interface: Identification of binding complexes, charge reversal, and detection limits. United States: N. p., 2021. Web. doi:10.1016/j.jcis.2021.10.052.
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Sthoer, Adrien, Adams, Ellen M., Sengupta, Sanghamitra, Corkery, Robert W., Allen, Heather C., & Tyrode, Eric C. La3+ and Y3+ interactions with the carboxylic acid moiety at the liquid/vapor interface: Identification of binding complexes, charge reversal, and detection limits. United States. https://doi.org/10.1016/j.jcis.2021.10.052
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Sthoer, Adrien, Adams, Ellen M., Sengupta, Sanghamitra, Corkery, Robert W., Allen, Heather C., and Tyrode, Eric C. Fri . "La3+ and Y3+ interactions with the carboxylic acid moiety at the liquid/vapor interface: Identification of binding complexes, charge reversal, and detection limits". United States. https://doi.org/10.1016/j.jcis.2021.10.052. https://www.osti.gov/servlets/purl/1830737.
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@article{osti_1830737,
title = {La3+ and Y3+ interactions with the carboxylic acid moiety at the liquid/vapor interface: Identification of binding complexes, charge reversal, and detection limits},
author = {Sthoer, Adrien and Adams, Ellen M. and Sengupta, Sanghamitra and Corkery, Robert W. and Allen, Heather C. and Tyrode, Eric C.},
abstractNote = {Specific interactions of yttrium and lanthanum ions with a fatty acid Langmuir monolayer were investigated using vibrational sum frequency spectroscopy. The trivalent ions were shown to interact with the charged form of the carboxylic acid group from nanomolar concentrations (<300 nM). Analysis of the spectral features from both the symmetric and the asymmetric carboxylate modes reveals the presence of at least three distinct coordination structures linked to specific binding configurations. Although the same species were identified for both La3+ and Y3+, they display a different concentration dependence, highlighting the ion-specificity of the interaction. From the analysis of the response of interfacial water molecules, the reversal of the surface charge, as well as the formation of yttrium hydroxide complexes, were detected upon increasing the amount of salt in solution. The binding interaction and kinetics of absorption are sensitive to the solution pH, showing a distinct ion speciation in the interfacial region when compared to the bulk. Changing the subphase pH or adding a monovalent background electrolyte that promotes deprotonation of the carboxylic acid headgroup could further improve the detection limit of La3+ and Y3+ to concentrations < 100 nM. These findings demonstrate that nM concentrations of trace metals contaminants, typically found on monovalent salts, can significantly influence the binding structure and kinetics in Langmuir monolayers.},
doi = {10.1016/j.jcis.2021.10.052},
journal = {Journal of Colloid and Interface Science},
number = Part 2,
volume = 608,
place = {United States},
year = {Fri Oct 15 00:00:00 EDT 2021},
month = {Fri Oct 15 00:00:00 EDT 2021}
}
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Works referenced in this record:

Influence of Multivalent Metal Ions on the Monolayer and Multilayer Properties of Some Unsaturated Fatty Acids
journal, November 1995

Effects of Hofmeister Anions on DPPC Langmuir Monolayers at the Air−Water Interface
journal, August 2004

  • Aroti, A.; Leontidis, E.; Maltseva, E.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 39
  • DOI: 10.1021/jp0481512

Breakdown of the Gouy−Chapman Model for Highly Charged Langmuir Monolayers:  Counterion Size Effect
journal, May 2006

  • Shapovalov, Vladimir L.; Brezesinski, Gerald
  • The Journal of Physical Chemistry B, Vol. 110, Issue 20
  • DOI: 10.1021/jp056801b

Effect of Ions on a Dipalmitoyl Phosphatidylcholine Bilayer. A Molecular Dynamics Simulation Study
journal, January 2008

  • Cordomí, Arnau; Edholm, Olle; Perez, Juan J.
  • The Journal of Physical Chemistry B, Vol. 112, Issue 5
  • DOI: 10.1021/jp073897w

Effects of Divalent Cations on Phase Behavior and Structure of a Zwitterionic Phospholipid (DMPC) Monolayer at the Air−Water Interface
journal, December 2009

  • Kewalramani, Sumit; Hlaing, Htay; Ocko, Benjamin M.
  • The Journal of Physical Chemistry Letters, Vol. 1, Issue 2
  • DOI: 10.1021/jz9002873

Effect of cation enrichment on dipalmitoylphosphatidylcholine (DPPC) monolayers at the air-water interface
journal, September 2016

  • Adams, Ellen M.; Casper, Clayton B.; Allen, Heather C.
  • Journal of Colloid and Interface Science, Vol. 478
  • DOI: 10.1016/j.jcis.2016.06.016

Identification of an organic coating on marine aerosol particles by TOF-SIMS
journal, January 2002

Essentiality of fatty acids
journal, January 1999

Analysis of Organic Anionic Surfactants in Fine and Coarse Fractions of Freshly Emitted Sea Spray Aerosol
journal, February 2016

  • Cochran, Richard E.; Laskina, Olga; Jayarathne, Thilina
  • Environmental Science & Technology, Vol. 50, Issue 5
  • DOI: 10.1021/acs.est.5b04053

Diagnosis of the nature of carboxylate coordination from the direction of shifts of carbonoxygen stretching frequencies
journal, October 1985

Structure of rare earth carboxylates in dimeric and polymeric forms
journal, December 1988

FT-IR Characterization of Metal Acetates in Aqueous Solution
journal, March 1989

The Effects of Divalent Ions on Langmuir Monolayer and Subphase Structure:  A Grazing-Incidence Diffraction and Bragg Rod Study
journal, November 2001

  • Kmetko, Jan; Datta, Alokmay; Evmenenko, Guennadi
  • The Journal of Physical Chemistry B, Vol. 105, Issue 44
  • DOI: 10.1021/jp0122169

Binding of Mg 2+ and Ca 2+ to Palmitic Acid and Deprotonation of the COOH Headgroup Studied by Vibrational Sum Frequency Generation Spectroscopy
journal, December 2010

  • Tang, Cheng Y.; Huang, Zishuai; Allen, Heather C.
  • The Journal of Physical Chemistry B, Vol. 114, Issue 51
  • DOI: 10.1021/jp105472e

Designated Drivers: The Differing Roles of Divalent Metal Ions in Surfactant Adsorption at the Oil–Water Interface
journal, December 2013

  • Robertson, Ellen J.; Beaman, Daniel K.; Richmond, Geraldine L.
  • Langmuir, Vol. 29, Issue 50
  • DOI: 10.1021/la403665n

Influence of Salt Purity on Na + and Palmitic Acid Interactions
journal, October 2013

  • Huang, Zishuai; Hua, Wei; Verreault, Dominique
  • The Journal of Physical Chemistry A, Vol. 117, Issue 50
  • DOI: 10.1021/jp406690p

Molecular insight into carboxylic acid–alkali metal cations interactions: reversed affinities and ion-pair formation revealed by non-linear optics and simulations
journal, January 2019

  • Sthoer, Adrien; Hladílková, Jana; Lund, Mikael
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 21
  • DOI: 10.1039/C9CP00398C

Impact of Salt Purity on Interfacial Water Organization Revealed by Conventional and Heterodyne-Detected Vibrational Sum Frequency Generation Spectroscopy
journal, September 2013

  • Hua, Wei; Verreault, Dominique; Adams, Ellen M.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 38
  • DOI: 10.1021/jp408146t

Specific Ion Effects of Trivalent Cations on the Structure and Charging State of β-Lactoglobulin Adsorption Layers
journal, August 2019

Interplay of pH and Binding of Multivalent Metal Ions: Charge Inversion and Reentrant Condensation in Protein Solutions
journal, April 2013

  • Roosen-Runge, Felix; Heck, Benjamin S.; Zhang, Fajun
  • The Journal of Physical Chemistry B, Vol. 117, Issue 18
  • DOI: 10.1021/jp401874t

Bulk Phase Behavior vs Interface Adsorption: Specific Multivalent Cation and Anion Effects on BSA Interactions
journal, January 2021

Molecular mechanism of charge inversion revealed by polar orientation of interfacial water molecules: A heterodyne-detected vibrational sum frequency generation study
journal, July 2018

  • Sartin, Matthew M.; Sung, Woongmo; Nihonyanagi, Satoshi
  • The Journal of Chemical Physics, Vol. 149, Issue 2
  • DOI: 10.1063/1.5024310

Ionic Specificity in pH Regulated Charged Interfaces: Fe 3+ versus La 3+
journal, October 2011

  • Wang, Wenjie; Park, Rebecca Y.; Meyer, David H.
  • Langmuir, Vol. 27, Issue 19
  • DOI: 10.1021/la201880g

Ion-Specific Induced Charges at Aqueous Soft Interfaces
journal, February 2011

Interaction of Arachidic Acid Langmuir Monolayers with Trivalent Ions La3+ and Fe3+ Studied by Vibrational Sum-Frequency Spectroscopy
journal, January 2018

Binding of trivalent ions on fatty acid Langmuir monolayer: Fe 3+ versus La 3+
journal, October 2018

  • Sung, Woongmo; Krem, Sona; Kim, Doseok
  • The Journal of Chemical Physics, Vol. 149, Issue 16
  • DOI: 10.1063/1.5028296

Lanthanide-Based Luminescent Hybrid Materials
journal, September 2009

Vibrational Sum Frequency Spectroscopy Studies at Solid/Liquid Interfaces: Influence of the Experimental Geometry in the Spectral Shape and Enhancement
journal, October 2012

  • Liljeblad, Jonathan F. D.; Tyrode, Eric
  • The Journal of Physical Chemistry C, Vol. 116, Issue 43
  • DOI: 10.1021/jp306838a

Quantitative analysis of monolayer composition by sum-frequency vibrational spectroscopy
journal, August 1991

  • Bain, Colin D.; Davies, Paul B.; Ong, T. Hui.
  • Langmuir, Vol. 7, Issue 8
  • DOI: 10.1021/la00056a003

The elusive silica/water interface: isolated silanols under water as revealed by vibrational sum frequency spectroscopy
journal, January 2017

  • Dalstein, Laetitia; Potapova, Elizaveta; Tyrode, Eric
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 16
  • DOI: 10.1039/C7CP01507K

Mesophases and crystalline phases in fatty acid monolayers
journal, March 1991

  • Kenn, R. M.; Boehm, C.; Bibo, A. M.
  • The Journal of Physical Chemistry, Vol. 95, Issue 5
  • DOI: 10.1021/j100158a034

Structure and phase transitions in Langmuir monolayers
journal, April 1999

  • Kaganer, Vladimir M.; Möhwald, Helmuth; Dutta, Pulak
  • Reviews of Modern Physics, Vol. 71, Issue 3
  • DOI: 10.1103/RevModPhys.71.779

Charging of Carboxylic Acid Monolayers with Monovalent Ions at Low Ionic Strengths: Molecular Insight Revealed by Vibrational Sum Frequency Spectroscopy
journal, November 2018

Langmuir-Blodgett deposition of yttrium arachidate
journal, September 1993

Monolayer properties of fatty acids
journal, July 1967

Textures and phase transitions in Langmuir monolayers of fatty acids. A comparative Brewster angle microscope and polarized fluorescence microscope study
journal, December 1994

  • Rivière, S.; Hénon, S.; Meunier, J.
  • The Journal of Chemical Physics, Vol. 101, Issue 11
  • DOI: 10.1063/1.467993

2D−3D Transformations of Amphiphilic Monolayers Influenced by Intermolecular Interactions:  A Brewster Angle Microscopy Study
journal, January 1996

  • Angelova, A.; Vollhardt, D.; Ionov, R.
  • The Journal of Physical Chemistry, Vol. 100, Issue 25
  • DOI: 10.1021/jp960417k

Effect of Ionic Repulsion among Hydrophilic Groups on Aggregation Structure of Fatty Acid Monolayer on the Water Surface
journal, April 1997

  • Oishi, Yushi; Takashima, Yoshinari; Suehiro, Kazuaki
  • Langmuir, Vol. 13, Issue 9
  • DOI: 10.1021/la960215f

Fatty acid monolayer dissociation and collapse: Effect of pH and cations
journal, July 2008

  • Kundu, Sarathi; Langevin, Dominique
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 325, Issue 1-2
  • DOI: 10.1016/j.colsurfa.2008.04.037

Arachidic Acid Monolayers at High pH of the Aqueous Subphase:  Studies of Counterion Bonding
journal, August 2000

  • Fainerman, V. B.; Vollhardt, D.; Johann, R.
  • Langmuir, Vol. 16, Issue 20
  • DOI: 10.1021/la0003903

Interactions of Na + Cations with a Highly Charged Fatty Acid Langmuir Monolayer: Molecular Description of the Phase Transition
journal, August 2019

Infrared Spectra of Metallic Complexes. IV. Comparison of the Infrared Spectra of Unidentate and Bidentate Metallic Complexes
journal, September 1957

  • Nakamoto, Kazuo; Fujita, Junnosuke; Tanaka, Shizuo
  • Journal of the American Chemical Society, Vol. 79, Issue 18
  • DOI: 10.1021/ja01575a020

Molecular-level origin of the carboxylate head group response to divalent metal ion complexation at the air–water interface
journal, July 2019

  • Denton, Joanna K.; Kelleher, Patrick J.; Johnson, Mark A.
  • Proceedings of the National Academy of Sciences, Vol. 116, Issue 30
  • DOI: 10.1073/pnas.1818600116

Ion Pairing
journal, November 2006

  • Marcus, Yizhak; Hefter, Glenn
  • Chemical Reviews, Vol. 106, Issue 11
  • DOI: 10.1021/cr040087x

X-ray and spectroscopic investigations of the structure of yttrium acetate tetrahydrate
journal, July 1991

Raman Study of the Coordination Structure of a Rare Earth−Acetate Complex in Water
journal, June 2007

  • Takekiyo, Takahiro; Yoshimura, Yukihiro
  • The Journal of Physical Chemistry A, Vol. 111, Issue 27
  • DOI: 10.1021/jp070521+

Structure and Mesomorphism of Neodymium(III) Alkanoates
journal, December 2000

  • Binnemans, Koen; Jongen, Liesbet; Bromant, Claudia
  • Inorganic Chemistry, Vol. 39, Issue 26
  • DOI: 10.1021/ic000470u

Crystal structure of lanthanum(III) butyrate monohydrate
journal, July 2001

Synthesis, crystal structure and thermal decomposition of [La2(CH3CH2COO)6·(H2O)3]·3.5H2O precursor for high-k La2O3 thin films deposition
journal, September 2010

Yttrium tris-propionate monohydrate: Synthesis, crystal structure, and thermal stability
journal, August 2014

  • Martynova, I. A.; Tsymbarenko, D. M.; Kuz’mina, N. P.
  • Russian Journal of Coordination Chemistry, Vol. 40, Issue 8
  • DOI: 10.1134/S1070328414080077

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

Second Harmonic and Sum-Frequency Generation from Aqueous Interfaces Is Modulated by Interference
journal, April 2016

  • Gonella, Grazia; Lütgebaucks, Cornelis; de Beer, Alex G. F.
  • The Journal of Physical Chemistry C, Vol. 120, Issue 17
  • DOI: 10.1021/acs.jpcc.5b12453

Unveiling Microscopic Structures of Charged Water Interfaces by Surface-Specific Vibrational Spectroscopy
journal, January 2016

Bulk Contributions Modulate the Sum-Frequency Generation Spectra of Water on Model Sea-Spray Aerosols
journal, July 2018

Probing Charged Aqueous Interfaces Near Critical Angles: Effect of Varying Coherence Length
journal, June 2019

Adsorption of CTAB on Hydrophilic Silica Studied by Linear and Nonlinear Optical Spectroscopy
journal, December 2008

  • Tyrode, Eric; Rutland, Mark W.; Bain, Colin D.
  • Journal of the American Chemical Society, Vol. 130, Issue 51
  • DOI: 10.1021/ja805169z

Direct and Reverse Hofmeister Effects on Interfacial Water Structure
journal, June 2012

  • Flores, Sarah C.; Kherb, Jaibir; Cremer, Paul S.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 27
  • DOI: 10.1021/jp3029352

In-situ spectroscopic investigations of surfactantadsorption and water structure at the CaF 2 /aqueous solution interface
journal, January 2004

  • Becraft, Kevin A.; Moore, Fred G.; Richmond, Geraldine L.
  • Phys. Chem. Chem. Phys., Vol. 6, Issue 8
  • DOI: 10.1039/B313513F

Liquid flow along a solid surface reversibly alters interfacial chemistry
journal, June 2014

Overcharging, charge reversal: Chemistry or physics?
journal, December 2006

Charge Inversion and Ion−Ion Correlation Effects at the Mercury/Aqueous MgSO 4 Interface: Toward the Solution of a Long-Standing Issue
journal, January 2010

  • Wernersson, Erik; Kjellander, Roland; Lyklema, Johannes
  • The Journal of Physical Chemistry C, Vol. 114, Issue 4
  • DOI: 10.1021/jp906759e

Structure of the Silica/Divalent Electrolyte Interface: Molecular Insight into Charge Inversion with Increasing pH
journal, November 2020

  • Rashwan, Mokhtar; Rehl, Benjamin; Sthoer, Adrien
  • The Journal of Physical Chemistry C, Vol. 124, Issue 49
  • DOI: 10.1021/acs.jpcc.0c09747

Structures and Charging of α-Alumina (0001)/Water Interfaces Studied by Sum-Frequency Vibrational Spectroscopy
journal, June 2008

  • Zhang, Luning; Tian, Chuanshan; Waychunas, Glenn A.
  • Journal of the American Chemical Society, Vol. 130, Issue 24
  • DOI: 10.1021/ja8011116

In Situ Vibrational Spectroscopic Studies of the CaF 2 /H 2 O Interface
journal, December 2001

Identifying Eigen-like hydrated protons at negatively charged interfaces
journal, January 2020

Two-Step Adsorption of PtCl 6 2– Complexes at a Charged Langmuir Monolayer: Role of Hydration and Ion Correlations
journal, November 2017

  • Uysal, Ahmet; Rock, William; Qiao, Baofu
  • The Journal of Physical Chemistry C, Vol. 121, Issue 45
  • DOI: 10.1021/acs.jpcc.7b09350
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