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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 = {2021},
month = {10}
}
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