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

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

Journal Article · Wed Mar 23 00:00:00 EDT 2016 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.6b02851· OSTI ID:1245397

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)

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.

View Accepted Manuscript (DOE)

Research Organization:: 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 Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

OSTI ID:: 1245397

Alternate ID(s):: OSTI ID: 1354469

Report Number(s):: BNL--111991-2016-JA; KC0403020

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 10 Vol. 67; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (34)

Synthesis and Structure of Ultrathin Aluminosilicate Films Stacchiola, Dario; Kaya, Sarp; Weissenrieder, Jonas Angewandte Chemie International Edition, Vol. 45, Issue 45 https://doi.org/10.1002/anie.200602670	journal	November 2006
Visualizing Chemical Reactions Confined under Graphene Mu, Rentao; Fu, Qiang; Jin, Li Angewandte Chemie International Edition, Vol. 51, Issue 20 https://doi.org/10.1002/anie.201200413	journal	April 2012
Modeling Zeolites with Metal-Supported Two-Dimensional Aluminosilicate Films Boscoboinik, Jorge Anibal; Yu, Xin; Yang, Bing Angewandte Chemie International Edition, Vol. 51, Issue 24 https://doi.org/10.1002/anie.201201319	journal	April 2012
2D Zeolite Coatings: Langmuir-Schaefer Deposition of 3 nm Thick MFI Zeolite Nanosheets Rangnekar, Neel; Shete, Meera; Agrawal, Kumar Varoon Angewandte Chemie International Edition, Vol. 54, Issue 22 https://doi.org/10.1002/anie.201411791	journal	April 2015
Self-Pillared, Single-Unit-Cell Sn-MFI Zeolite Nanosheets and Their Use for Glucose and Lactose Isomerization Ren, Limin; Guo, Qiang; Kumar, Prashant Angewandte Chemie International Edition, Vol. 54, Issue 37 https://doi.org/10.1002/anie.201505334	journal	July 2015
Ultrathin Silica Films: The Atomic Structure of Two-Dimensional Crystals and Glasses Büchner, Christin; Lichtenstein, Leonid; Yu, Xin Chemistry - A European Journal, Vol. 20, Issue 30 https://doi.org/10.1002/chem.201402452	journal	July 2014
Exploring Zeolite Chemistry with the Tools of Surface Science: Challenges, Opportunities, and Limitations Boscoboinik, J. Anibal; Shaikhutdinov, Shamil Catalysis Letters, Vol. 144, Issue 12 https://doi.org/10.1007/s10562-014-1369-3	journal	September 2014
Adsorbate induced reconstruction by strong chemisorption: Ru(001)p(2×2)-O Lindroos, M.; Pfnür, H.; Held, G. Surface Science, Vol. 222, Issue 2-3 https://doi.org/10.1016/0039-6028(89)90371-3	journal	November 1989
Oxygen induced reconstruction of a close-packed surface: A LEED IV study on Ru(001)-p(2 × 1)O Pfnür, H.; Held, G.; Lindroos, M. Surface Science, Vol. 220, Issue 1 https://doi.org/10.1016/0039-6028(89)90462-7	journal	October 1989
On the origin of the Ru-3d5/2 satellite feature from RuO2() Over, H.; Seitsonen, A. P.; Lundgren, E. Surface Science, Vol. 504 https://doi.org/10.1016/S0039-6028(01)01979-3	journal	April 2002
Observation of a novel high density 3O(2 × 2) structure on Ru(001) Kostov, K. L.; Gsell, M.; Jakob, P. Surface Science, Vol. 394, Issue 1-3 https://doi.org/10.1016/S0039-6028(97)00787-5	journal	December 1997
Catalytically active states of Ru(0001) catalyst in CO oxidation reaction Blume, R.; Havecker, M.; Zafeiratos, S. Journal of Catalysis, Vol. 239, Issue 2 https://doi.org/10.1016/j.jcat.2006.02.019	journal	April 2006
CO adsorption and dissociation on Ru(0001) at elevated pressures Starr, David E.; Bluhm, Hendrik Surface Science, Vol. 608 https://doi.org/10.1016/j.susc.2012.10.014	journal	February 2013
Facile oxygen intercalation between full layer graphene and Ru(0001) under ambient conditions Dong, Aiyi; Fu, Qiang; Wei, Mingming Surface Science, Vol. 634 https://doi.org/10.1016/j.susc.2014.10.008	journal	April 2015
Preparation of silica films on Ru(0001): A LEEM/PEEM study Klemm, H. W.; Peschel, G.; Madej, E. Surface Science, Vol. 643 https://doi.org/10.1016/j.susc.2015.05.017	journal	January 2016
Oxidation of the Ru(0001) surface covered by weakly bound, ultrathin silicate films Emmez, Emre; Anibal Boscoboinik, J.; Tenney, Samuel Surface Science, Vol. 646 https://doi.org/10.1016/j.susc.2015.06.019	journal	April 2016
CO adsorption on a silica bilayer supported on Ru(0001) Schlexer, Philomena; Pacchioni, Gianfranco; Włodarczyk, Radosław Surface Science, Vol. 648 https://doi.org/10.1016/j.susc.2015.10.027	journal	June 2016
Preparation and characterization of atomically flat and ordered silica films on a Pd(100) surface Zhang, Zhen; Jiang, Zhiquan; Yao, Yunxi Thin Solid Films, Vol. 516, Issue 12 https://doi.org/10.1016/j.tsf.2007.06.070	journal	April 2008
Nanoscale Origin of Mesoscale Roughening: Real-Time Tracking and Identification of Three Distinct Ruthenium Oxide Phases in Ruthenium Oxidation Flege, Jan Ingo; Herd, Benjamin; Goritzka, Jan ACS Nano, Vol. 9, Issue 8 https://doi.org/10.1021/acsnano.5b03393	journal	July 2015
Separation of Xylene Isomer Vapors with Oriented MFI Membranes Made by Seeded Growth Xomeritakis, George; Lai, Zhiping; Tsapatsis, Michael Industrial & Engineering Chemistry Research, Vol. 40, Issue 2 https://doi.org/10.1021/ie000613k	journal	January 2001
Chemistry under Cover: Tuning Metal−Graphene Interaction by Reactive Intercalation Sutter, Peter; Sadowski, Jerzy T.; Sutter, Eli A. Journal of the American Chemical Society, Vol. 132, Issue 23 https://doi.org/10.1021/ja102398n	journal	June 2010
Long-Term Passivation of Strongly Interacting Metals with Single-Layer Graphene Weatherup, Robert S.; D’Arsié, Lorenzo; Cabrero-Vilatela, Andrea Journal of the American Chemical Society, Vol. 137, Issue 45 https://doi.org/10.1021/jacs.5b08729	journal	November 2015
Permeation of a Single-Layer SiO ₂ Membrane and Chemistry in Confined Space Emmez, Emre; Yang, Bing; Shaikhutdinov, Shamil The Journal of Physical Chemistry C, Vol. 118, Issue 50 https://doi.org/10.1021/jp503253a	journal	June 2014
Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts Choi, Minkee; Na, Kyungsu; Kim, Jeongnam Nature, Vol. 461, Issue 7261, p. 246-249 https://doi.org/10.1038/nature08288	journal	September 2009
Quantification of thickness and wrinkling of exfoliated two-dimensional zeolite nanosheets Kumar, Prashant; Agrawal, Kumar Varoon; Tsapatsis, Michael Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8128	journal	May 2015
Insights into the gas phase oxidation of Ru(0001) on the mesoscopic scale using molecular oxygen Goritzka, Jan C.; Herd, Benjamin; Krause, Philipp P. T. Physical Chemistry Chemical Physics, Vol. 17, Issue 21 https://doi.org/10.1039/C4CP06010E	journal	January 2015
Thin silica films on Ru(0001): monolayer, bilayer and three-dimensional networks of [SiO4] tetrahedra Yang, Bing; Kaden, William E.; Yu, Xin Physical Chemistry Chemical Physics, Vol. 14, Issue 32 https://doi.org/10.1039/c2cp41355h	journal	January 2012
Growth of single-crystal SiO2 film on Ni(111) surface Kundu, Manisha; Murata, Yoshitada Applied Physics Letters, Vol. 80, Issue 11 https://doi.org/10.1063/1.1461052	journal	March 2002
Support effects on the atomic structure of ultrathin silica films on metals Yu, Xin; Yang, Bing; Anibal Boscoboinik, Jorge Applied Physics Letters, Vol. 100, Issue 15 https://doi.org/10.1063/1.3703609	journal	April 2012
Tuning the electronic structure of ultrathin crystalline silica films on Ru(0001) Włodarczyk, R.; Sierka, M.; Sauer, J. Physical Review B, Vol. 85, Issue 8 https://doi.org/10.1103/PhysRevB.85.085403	journal	February 2012
Growth and Structure of Crystalline Silica Sheet on Ru(0001) Löffler, D.; Uhlrich, J. J.; Baron, M. Physical Review Letters, Vol. 105, Issue 14 https://doi.org/10.1103/PhysRevLett.105.146104	journal	September 2010
Structure and Stability of a High-Coverage ( 1 × 1 ) Oxygen Phase on Ru(0001) Stampfl, C.; Schwegmann, S.; Over, H. Physical Review Letters, Vol. 77, Issue 16 https://doi.org/10.1103/PhysRevLett.77.3371	journal	October 1996
Atomic Structure of a Thin Silica Film on a Mo(112) Substrate: A Two-Dimensional Network of SiO 4 Tetrahedra Weissenrieder, J.; Kaya, S.; Lu, J. -L. Physical Review Letters, Vol. 95, Issue 7 https://doi.org/10.1103/PhysRevLett.95.076103	journal	August 2005
SURFACE CHEMISTRY: Oxidation of Metal Surfaces Over, H. Science, Vol. 297, Issue 5589 https://doi.org/10.1126/science.1077063	journal	September 2002

Cited By (7)

Ionization‐Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds Zhong, Jian‐Qiang; Wang, Mengen; Akter, Nusnin Advanced Functional Materials, Vol. 29, Issue 20 https://doi.org/10.1002/adfm.201806583	journal	March 2019
Energy Level Shifts at the Silica/Ru(0001) Heterojunction Driven by Surface and Interface Dipoles Wang, Mengen; Zhong, Jian-Qiang; Kestell, John Topics in Catalysis, Vol. 60, Issue 6-7 https://doi.org/10.1007/s11244-016-0704-x	journal	September 2016
X-ray Microscopy Jacobsen, Chris Cambridge University Press https://doi.org/10.1017/9781139924542	book	January 2019
Synchrotron-based ambient pressure X-ray photoelectron spectroscopy of hydrogen and helium Zhong, Jian-Qiang; Wang, Mengen; Hoffmann, William H. Applied Physics Letters, Vol. 112, Issue 9 https://doi.org/10.1063/1.5022479	journal	February 2018
X-ray microscopy Cosslett, V. E. Reports on Progress in Physics, Vol. 28, Issue 1 https://doi.org/10.1088/0034-4885/28/1/311	journal	July 1965
Chemistry in confined space through the eyes of surface science—2D porous materials Boscoboinik, J. Anibal Journal of Physics: Condensed Matter, Vol. 31, Issue 6 https://doi.org/10.1088/1361-648x/aaf2ce	journal	December 2018
X-ray microscopy Lider, V. V. Physics-Uspekhi, Vol. 60, Issue 2 https://doi.org/10.3367/ufne.2016.06.037830	journal	February 2017

Similar Records

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

Journal Article · Mon Jun 29 20:00:00 EDT 2015 · Surface Science · OSTI ID:1336055

Room-Temperature in Vacuo Chemisorption of Xenon Atoms on Ru(0001) under Interface Confinement

Journal Article · Sun May 05 20:00:00 EDT 2019 · Journal of Physical Chemistry. C · OSTI ID:1515149

Energy level shifts at the silica/Ru(0001) heterojunction driven by surface and interface dipoles

Journal Article · Sun Sep 11 20:00:00 EDT 2016 · Topics in Catalysis · OSTI ID:1328366

Related Subjects

36 MATERIALS SCIENCE

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

Citation Formats

References (34)

Cited By (7)

Similar Records

Related Subjects