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Calcite Surfaces Modified with Carboxylic Acids (C2 to C18): Layer Organization, Wettability, Stability, and Molecular Structural Properties
RISE Research Institutes of Sweden, Bioeconomy and Health, Material and Surface Design. KTH Royal Institute of Technology, Sweden.ORCID iD: 0000-0002-6181-1347
KTH Royal Institute of Technology, Sweden.
KTH Royal Institute of Technology, Sweden; Australian National University Department of Applied Mathematics, Australia.
RISE Research Institutes of Sweden, Bioeconomy and Health, Material and Surface Design.ORCID iD: 0000-0003-3695-1150
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2023 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 39, no 42, p. 14840-14852Article in journal (Refereed) Published
Abstract [en]

A fundamental understanding of the interactions between mineral surfaces and amphiphilic surface modification agents is needed for better control over the production and uses of mineral fillers. Here, we controlled the carboxylic acid layer formation conditions on calcite surfaces with high precision via vapor deposition. The properties of the resulting carboxylic acid layers were analyzed using surface-sensitive techniques, such as atomic force microscopy (AFM), contact angle measurements, angle resolved X-ray photoelectron spectroscopy (XPS), and vibrational sum-frequency spectroscopy. A low wettability was achieved with long hydrocarbon chain carboxylic acids such as stearic acid. The stearic acid layer formed by vapor deposition is initially patchy, but with increasing vapor exposure time, the patches grow and condense into a homogeneous layer with a thickness close to that expected for a monolayer as evaluated by AFM and XPS. The build-up process of the layer occurs more rapidly at higher temperatures due to the higher vapor pressure. The stability of the deposited fatty acid layer in the presence of a water droplet increases with the chain length and packing density in the adsorbed layer. Vibrational sum frequency spectroscopy data demonstrate that the stearic acid monolayers on calcite have their alkyl chains in an all-trans conformation and are anisotropically distributed on the plane of the surface, forming epitaxial monolayers. Vibrational spectra also show that the stearic acid molecules interact with the calcite surface through the carboxylic acid headgroup in both its protonated and deprotonated forms. The results presented provide new molecular insights into the properties of adsorbed carboxylic acid layers on calcite.

Place, publisher, year, edition, pages
2023. Vol. 39, no 42, p. 14840-14852
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Mechanical Engineering
Identifiers
URN: urn:nbn:se:ri:diva-67911DOI: 10.1021/acs.langmuir.3c01252Scopus ID: 2-s2.0-85175357225OAI: oai:DiVA.org:ri-67911DiVA, id: diva2:1814699
Note

This work was funded by Omya International AG. ET acknowledges support from the Swedish Research Council (VR).

Available from: 2023-11-27 Created: 2023-11-27 Last updated: 2024-02-28Bibliographically approved

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Wojas, NataliaErnstsson, MarieWallqvist, VivecaJärn, MikaelSwerin, Agne

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