Oxidation and reduction under cover: Chemistry at the confined space between ultra-thin nanoporous silicates and Ru(0001)
Abstract
The oxidation and reduction of Ru(0001) surfaces at the confined space between two-dimensional nanoporous silica frameworks and Ru(0001) have been investigated using synchrotron-based ambient pressure X-ray photoelectron spectroscopy (AP-XPS). The porous nature of the frameworks and the weak interaction between the silica and the ruthenium substrate allow oxygen and hydrogen molecules to go through the nanopores and react with the metal at the interface between the silica framework and the metal surface. In this work, three types of two-dimensional silica frameworks have been used to study their influence in the oxidation and reduction of the ruthenium surface at elevated pressures and temperatures. These frameworks are bilayer silica (0.5 nm thick), bilayer aluminosilicate (0.5 nm thick), and zeolite MFI nanosheets (3 nm thick). It is found that the silica frameworks stay essentially intact under these conditions, but they strongly affect the oxidation of ruthenium, with the 0.5 nm thick aluminosilicate bilayer completely inhibiting the oxidation. Furthermore, the latter is believed to be related to the lower chemisorbed oxygen content arising from electrostatic interactions between the negatively charged aluminosilicate framework and the Ru(0001) substrate.
- Authors:
-
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- National Synchrotron Light Source II, Upton, NY (United States)
- Univ. of Minnesota, Minneapolis, MN (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1245397
- Report Number(s):
- BNL-111991-2016-JA
Journal ID: ISSN 1932-7447; KC0403020
- Grant/Contract Number:
- SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 67; Journal Issue: 10; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
J. Anibal Boscoboinik, Zhong, Jian -Qiang, Kestell, John, Waluyo, Iradwikanari, Wilkins, Stuart, Mazzoli, Claudio, Barbour, Andi, Kaznatcheev, Konstantine, Shete, Meere, and Tsapatsis, Michael. Oxidation and reduction under cover: Chemistry at the confined space between ultra-thin nanoporous silicates and Ru(0001). United States: N. p., 2016.
Web. doi:10.1021/acs.jpcc.6b02851.
J. Anibal Boscoboinik, Zhong, Jian -Qiang, Kestell, John, Waluyo, Iradwikanari, Wilkins, Stuart, Mazzoli, Claudio, Barbour, Andi, Kaznatcheev, Konstantine, Shete, Meere, & Tsapatsis, Michael. Oxidation and reduction under cover: Chemistry at the confined space between ultra-thin nanoporous silicates and Ru(0001). United States. https://doi.org/10.1021/acs.jpcc.6b02851
J. Anibal Boscoboinik, Zhong, Jian -Qiang, Kestell, John, Waluyo, Iradwikanari, Wilkins, Stuart, Mazzoli, Claudio, Barbour, Andi, Kaznatcheev, Konstantine, Shete, Meere, and Tsapatsis, Michael. Wed .
"Oxidation and reduction under cover: Chemistry at the confined space between ultra-thin nanoporous silicates and Ru(0001)". United States. https://doi.org/10.1021/acs.jpcc.6b02851. https://www.osti.gov/servlets/purl/1245397.
@article{osti_1245397,
title = {Oxidation and reduction under cover: Chemistry at the confined space between ultra-thin nanoporous silicates and Ru(0001)},
author = {J. Anibal Boscoboinik and Zhong, Jian -Qiang and Kestell, John and Waluyo, Iradwikanari and Wilkins, Stuart and Mazzoli, Claudio and Barbour, Andi and Kaznatcheev, Konstantine and Shete, Meere and Tsapatsis, Michael},
abstractNote = {The oxidation and reduction of Ru(0001) surfaces at the confined space between two-dimensional nanoporous silica frameworks and Ru(0001) have been investigated using synchrotron-based ambient pressure X-ray photoelectron spectroscopy (AP-XPS). The porous nature of the frameworks and the weak interaction between the silica and the ruthenium substrate allow oxygen and hydrogen molecules to go through the nanopores and react with the metal at the interface between the silica framework and the metal surface. In this work, three types of two-dimensional silica frameworks have been used to study their influence in the oxidation and reduction of the ruthenium surface at elevated pressures and temperatures. These frameworks are bilayer silica (0.5 nm thick), bilayer aluminosilicate (0.5 nm thick), and zeolite MFI nanosheets (3 nm thick). It is found that the silica frameworks stay essentially intact under these conditions, but they strongly affect the oxidation of ruthenium, with the 0.5 nm thick aluminosilicate bilayer completely inhibiting the oxidation. Furthermore, the latter is believed to be related to the lower chemisorbed oxygen content arising from electrostatic interactions between the negatively charged aluminosilicate framework and the Ru(0001) substrate.},
doi = {10.1021/acs.jpcc.6b02851},
journal = {Journal of Physical Chemistry. C},
number = 10,
volume = 67,
place = {United States},
year = {Wed Mar 23 00:00:00 EDT 2016},
month = {Wed Mar 23 00:00:00 EDT 2016}
}
Web of Science
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