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Title: Unravelling the Chemical Influence of Water on the PMMA/Aluminum Oxide Hybrid Interface In Situ

Abstract

Understanding the stability of chemical interactions at the polymer/metal oxide interface under humid conditions is vital to understand the long-term durability of hybrid systems. Therefore, the interface of ultrathin PMMA films on native aluminum oxide, deposited by reactive adsorption, was studied. The characterization of the interface of the coated substrates was performed using ambient pressure X-ray photoelectron spectroscopy (APXPS), Fourier transform infrared spectroscopy in the Kretschmann geometry (ATR-FTIR Kretschmann) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). The formation of hydrogen bonds and carboxylate ionic bonds at the interface are observed. The formed ionic bond is stable up to 5 Torr water vapour pressure as shown by APXPS. However, when the coated samples are exposed to an excess of aqueous electrolyte, an increase in the amount of carboxylate bonds at the interface, as a result of hydrolysis of the methoxy group, is observed by ATR-FTIR Kretschmann. In conclusion, these observations, supported by ToF-SIMS spectra, lead to the proposal of an adsorption mechanism of PMMA on aluminum oxide, which shows the formation of methanol at the interface and the effect of water molecules on the different interfacial interactions.

Authors:
ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [3];  [3];  [2]; ORCiD logo [2]
  1. Vrije Univ. Brussel, Brussels, (Belgium). Dept. of Electrochemical and Surface Engineering (SURF); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  2. Vrije Univ. Brussel, Brussels, (Belgium). Dept. of Electrochemical and Surface Engineering (SURF)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  4. Delft Univ. of Technology (Netherlands). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOD; Research Foundation Flanders (FWO)
OSTI Identifier:
1419452
Grant/Contract Number:  
AC02-05CH11231; HDTRA11510005
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Pletincx, Sven, Marcoen, Kristof, Trotochaud, Lena, Fockaert, Laura-Lynn, Mol, Johannes M. C., Head, Ashley R., Karslioğlu, Osman, Bluhm, Hendrik, Terryn, Herman, and Hauffman, Tom. Unravelling the Chemical Influence of Water on the PMMA/Aluminum Oxide Hybrid Interface In Situ. United States: N. p., 2017. Web. doi:10.1038/s41598-017-13549-z.
Pletincx, Sven, Marcoen, Kristof, Trotochaud, Lena, Fockaert, Laura-Lynn, Mol, Johannes M. C., Head, Ashley R., Karslioğlu, Osman, Bluhm, Hendrik, Terryn, Herman, & Hauffman, Tom. Unravelling the Chemical Influence of Water on the PMMA/Aluminum Oxide Hybrid Interface In Situ. United States. doi:10.1038/s41598-017-13549-z.
Pletincx, Sven, Marcoen, Kristof, Trotochaud, Lena, Fockaert, Laura-Lynn, Mol, Johannes M. C., Head, Ashley R., Karslioğlu, Osman, Bluhm, Hendrik, Terryn, Herman, and Hauffman, Tom. Tue . "Unravelling the Chemical Influence of Water on the PMMA/Aluminum Oxide Hybrid Interface In Situ". United States. doi:10.1038/s41598-017-13549-z. https://www.osti.gov/servlets/purl/1419452.
@article{osti_1419452,
title = {Unravelling the Chemical Influence of Water on the PMMA/Aluminum Oxide Hybrid Interface In Situ},
author = {Pletincx, Sven and Marcoen, Kristof and Trotochaud, Lena and Fockaert, Laura-Lynn and Mol, Johannes M. C. and Head, Ashley R. and Karslioğlu, Osman and Bluhm, Hendrik and Terryn, Herman and Hauffman, Tom},
abstractNote = {Understanding the stability of chemical interactions at the polymer/metal oxide interface under humid conditions is vital to understand the long-term durability of hybrid systems. Therefore, the interface of ultrathin PMMA films on native aluminum oxide, deposited by reactive adsorption, was studied. The characterization of the interface of the coated substrates was performed using ambient pressure X-ray photoelectron spectroscopy (APXPS), Fourier transform infrared spectroscopy in the Kretschmann geometry (ATR-FTIR Kretschmann) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). The formation of hydrogen bonds and carboxylate ionic bonds at the interface are observed. The formed ionic bond is stable up to 5 Torr water vapour pressure as shown by APXPS. However, when the coated samples are exposed to an excess of aqueous electrolyte, an increase in the amount of carboxylate bonds at the interface, as a result of hydrolysis of the methoxy group, is observed by ATR-FTIR Kretschmann. In conclusion, these observations, supported by ToF-SIMS spectra, lead to the proposal of an adsorption mechanism of PMMA on aluminum oxide, which shows the formation of methanol at the interface and the effect of water molecules on the different interfacial interactions.},
doi = {10.1038/s41598-017-13549-z},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {Tue Oct 17 00:00:00 EDT 2017},
month = {Tue Oct 17 00:00:00 EDT 2017}
}

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