Oxidation and reduction under cover: Chemistry at the confined space between ultra-thin nanoporous silicates and Ru(0001)

Zhong, Jian -Qiang; Kestell, John; Waluyo, Iradwikanari; Wilkins, Stuart; Mazzoli, Claudio; Barbour, Andi; Kaznatcheev, Konstantine; Shete, Meere; Tsapatsis, Michael

doi:10.1021/acs.jpcc.6b02851

Title: 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:

Zhong, Jian -Qiang ^[1]; Kestell, John ^[1]; Waluyo, Iradwikanari ^[2]; Wilkins, Stuart ^[2]; Mazzoli, Claudio ^[2]; Barbour, Andi ^[2]; Kaznatcheev, Konstantine ^[2]; Shete, Meere ^[3]; Tsapatsis, Michael ^[3]

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:: Wed Mar 23 00:00:00 EDT 2016

Research Org.:: Brookhaven National Lab. (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:: Journal Article: 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.

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                    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

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                    J. Anibal Boscoboinik, Zhong, Jian -Qiang, Kestell, John, Waluyo, Iradwikanari, Wilkins, Stuart, Mazzoli, Claudio, Barbour, Andi, Kaznatcheev, Konstantine, Shete, Meere, and Tsapatsis, Michael. 2016.  
        "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.

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@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},

  url          = {https://www.osti.gov/biblio/1245397},
  journal      = {Journal of Physical Chemistry. C},

  issn         = {1932-7447},

  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}

}

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Works referencing / citing this record:

Ionization‐Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds
journal, March 2019

Zhong, Jian‐Qiang; Wang, Mengen; Akter, Nusnin
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Title: Oxidation and reduction under cover: Chemistry at the confined space between ultra-thin nanoporous silicates and Ru(0001)

Abstract

Citation Formats

Chemistry under Cover: Tuning Metal−Graphene Interaction by Reactive Intercalation journal, June 2010

Facile oxygen intercalation between full layer graphene and Ru(0001) under ambient conditions journal, April 2015

Visualizing Chemical Reactions Confined under Graphene journal, April 2012

Long-Term Passivation of Strongly Interacting Metals with Single-Layer Graphene journal, November 2015

Exploring Zeolite Chemistry with the Tools of Surface Science: Challenges, Opportunities, and Limitations journal, September 2014

Ultrathin Silica Films: The Atomic Structure of Two-Dimensional Crystals and Glasses journal, July 2014

Atomic Structure of a Thin Silica Film on a Mo(112) Substrate: A Two-Dimensional Network of SiO 4 Tetrahedra journal, August 2005

Synthesis and Structure of Ultrathin Aluminosilicate Films journal, November 2006

Growth of single-crystal SiO2 film on Ni(111) surface journal, March 2002

Preparation and characterization of atomically flat and ordered silica films on a Pd(100) surface journal, April 2008

Support effects on the atomic structure of ultrathin silica films on metals journal, April 2012

Modeling Zeolites with Metal-Supported Two-Dimensional Aluminosilicate Films journal, April 2012

Thin silica films on Ru(0001): monolayer, bilayer and three-dimensional networks of [SiO4] tetrahedra journal, January 2012

CO adsorption on a silica bilayer supported on Ru(0001) journal, June 2016

Oxidation of the Ru(0001) surface covered by weakly bound, ultrathin silicate films journal, April 2016

Permeation of a Single-Layer SiO 2 Membrane and Chemistry in Confined Space journal, June 2014

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2D Zeolite Coatings: Langmuir-Schaefer Deposition of 3 nm Thick MFI Zeolite Nanosheets journal, April 2015

Separation of Xylene Isomer Vapors with Oriented MFI Membranes Made by Seeded Growth journal, January 2001

Self-Pillared, Single-Unit-Cell Sn-MFI Zeolite Nanosheets and Their Use for Glucose and Lactose Isomerization journal, July 2015

Adsorbate induced reconstruction by strong chemisorption: Ru(001)p(2×2)-O journal, November 1989

Oxygen induced reconstruction of a close-packed surface: A LEED IV study on Ru(001)-p(2 × 1)O journal, October 1989

Observation of a novel high density 3O(2 × 2) structure on Ru(001) journal, December 1997

Structure and Stability of a High-Coverage ( 1 × 1 ) Oxygen Phase on Ru(0001) journal, October 1996

Catalytically active states of Ru(0001) catalyst in CO oxidation reaction journal, April 2006

CO adsorption and dissociation on Ru(0001) at elevated pressures journal, February 2013

Preparation of silica films on Ru(0001): A LEEM/PEEM study journal, January 2016

On the origin of the Ru-3d5/2 satellite feature from RuO2() journal, April 2002

Nanoscale Origin of Mesoscale Roughening: Real-Time Tracking and Identification of Three Distinct Ruthenium Oxide Phases in Ruthenium Oxidation journal, July 2015

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SURFACE CHEMISTRY: Oxidation of Metal Surfaces journal, September 2002

Ionization‐Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds journal, March 2019

Synchrotron-based ambient pressure X-ray photoelectron spectroscopy of hydrogen and helium journal, February 2018

Chemistry in confined space through the eyes of surface science—2D porous materials journal, December 2018

Energy Level Shifts at the Silica/Ru(0001) Heterojunction Driven by Surface and Interface Dipoles journal, September 2016

X-ray microscopy journal, July 1965

Chemistry under Cover: Tuning Metal−Graphene Interaction by Reactive Intercalation
journal, June 2010

Facile oxygen intercalation between full layer graphene and Ru(0001) under ambient conditions
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Visualizing Chemical Reactions Confined under Graphene
journal, April 2012

Long-Term Passivation of Strongly Interacting Metals with Single-Layer Graphene
journal, November 2015

Exploring Zeolite Chemistry with the Tools of Surface Science: Challenges, Opportunities, and Limitations
journal, September 2014

Ultrathin Silica Films: The Atomic Structure of Two-Dimensional Crystals and Glasses
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journal, August 2005

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journal, March 2002

Preparation and characterization of atomically flat and ordered silica films on a Pd(100) surface
journal, April 2008

Support effects on the atomic structure of ultrathin silica films on metals
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Modeling Zeolites with Metal-Supported Two-Dimensional Aluminosilicate Films
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Thin silica films on Ru(0001): monolayer, bilayer and three-dimensional networks of [SiO4] tetrahedra
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CO adsorption on a silica bilayer supported on Ru(0001)
journal, June 2016

Oxidation of the Ru(0001) surface covered by weakly bound, ultrathin silicate films
journal, April 2016

Permeation of a Single-Layer SiO ₂ Membrane and Chemistry in Confined Space
journal, June 2014

Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts
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2D Zeolite Coatings: Langmuir-Schaefer Deposition of 3 nm Thick MFI Zeolite Nanosheets
journal, April 2015

Separation of Xylene Isomer Vapors with Oriented MFI Membranes Made by Seeded Growth
journal, January 2001

Self-Pillared, Single-Unit-Cell Sn-MFI Zeolite Nanosheets and Their Use for Glucose and Lactose Isomerization
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Adsorbate induced reconstruction by strong chemisorption: Ru(001)p(2×2)-O
journal, November 1989

Oxygen induced reconstruction of a close-packed surface: A LEED IV study on Ru(001)-p(2 × 1)O
journal, October 1989

Observation of a novel high density 3O(2 × 2) structure on Ru(001)
journal, December 1997

Structure and Stability of a High-Coverage $(1 \times 1)$ Oxygen Phase on Ru(0001)
journal, October 1996

Catalytically active states of Ru(0001) catalyst in CO oxidation reaction
journal, April 2006

CO adsorption and dissociation on Ru(0001) at elevated pressures
journal, February 2013

Preparation of silica films on Ru(0001): A LEEM/PEEM study
journal, January 2016

On the origin of the Ru-3d5/2 satellite feature from RuO2()
journal, April 2002

Nanoscale Origin of Mesoscale Roughening: Real-Time Tracking and Identification of Three Distinct Ruthenium Oxide Phases in Ruthenium Oxidation
journal, July 2015

Quantification of thickness and wrinkling of exfoliated two-dimensional zeolite nanosheets
journal, May 2015

SURFACE CHEMISTRY: Oxidation of Metal Surfaces
journal, September 2002

Ionization‐Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds
journal, March 2019

Synchrotron-based ambient pressure X-ray photoelectron spectroscopy of hydrogen and helium
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Chemistry in confined space through the eyes of surface science—2D porous materials
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Energy Level Shifts at the Silica/Ru(0001) Heterojunction Driven by Surface and Interface Dipoles
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X-ray microscopy
journal, July 1965