Reversible Formation of Silanol Groups in Two-Dimensional Siliceous Nanomaterials under Mild Hydrothermal Conditions
Abstract
Monitoring the effects of mild hydrothermal conditions, in situ, on siliceous materials remains challenging using surface science techniques, which often require electrically conductive substrates. The emergence of two-dimensional (2-D) siliceous nanomaterials deposited on metal single crystals overcomes this limitation. Here, we use infrared reflection absorption spectroscopy (IRRAS) to study the effects of mild hydrothermal conditions, in situ, on 2-D model systems, namely, all-Si MFI nanosheets supported on Au(111) and a polymorphous bilayer silicate supported on Ru(0001). We find that the formation of silanol groups (SiOH) occurs at 473 and 573 K under a H2O pressure of 3 mbar in the MFI nanosheets, but not in the polymorphous bilayer silicate. The effects of mild hydrothermal conditions are reversible in the MFI nanosheets and do not result in framework degradation. Implications shown here provide a fundamental understanding of the impact of mild hydrothermal conditions on the 2-D siliceous nanomaterials and serve as a starting point when considering these effects on three-dimensional (3-D) ones.
- Authors:
-
- Univ. of Delaware, Newark, DE (United States)
- Univ. of Minnesota, Minneapolis, MN (United States); Chonnam National Univ., Gwangju (Korea, Republic of)
- Catalysis Center for Energy Innovation, University of Delaware, 221 Academy Street, Newark, Delaware 19716 United States
- Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Univ. of Delaware, Newark, DE (United States); Univ. of Minnesota, Minneapolis, MN (United States); Johns Hopkins Univ., Baltimore, MD (United States)
- Univ. of Delaware, Newark, DE (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1670664
- Report Number(s):
- BNL-219914-2020-JAAM
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- SC0012704; SC0001004
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 124; Journal Issue: 33; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY
Citation Formats
Norton, Angela M., Kim, Donghun, Zheng, Weiqing, Akter, Nusnin, Xu, Yixin, Tenney, Samuel A., Vlachos, Dionisios G., Tsapatsis, Michael, and Boscoboinik, J. Anibal. Reversible Formation of Silanol Groups in Two-Dimensional Siliceous Nanomaterials under Mild Hydrothermal Conditions. United States: N. p., 2020.
Web. doi:10.1021/acs.jpcc.0c03875.
Norton, Angela M., Kim, Donghun, Zheng, Weiqing, Akter, Nusnin, Xu, Yixin, Tenney, Samuel A., Vlachos, Dionisios G., Tsapatsis, Michael, & Boscoboinik, J. Anibal. Reversible Formation of Silanol Groups in Two-Dimensional Siliceous Nanomaterials under Mild Hydrothermal Conditions. United States. https://doi.org/10.1021/acs.jpcc.0c03875
Norton, Angela M., Kim, Donghun, Zheng, Weiqing, Akter, Nusnin, Xu, Yixin, Tenney, Samuel A., Vlachos, Dionisios G., Tsapatsis, Michael, and Boscoboinik, J. Anibal. Sun .
"Reversible Formation of Silanol Groups in Two-Dimensional Siliceous Nanomaterials under Mild Hydrothermal Conditions". United States. https://doi.org/10.1021/acs.jpcc.0c03875. https://www.osti.gov/servlets/purl/1670664.
@article{osti_1670664,
title = {Reversible Formation of Silanol Groups in Two-Dimensional Siliceous Nanomaterials under Mild Hydrothermal Conditions},
author = {Norton, Angela M. and Kim, Donghun and Zheng, Weiqing and Akter, Nusnin and Xu, Yixin and Tenney, Samuel A. and Vlachos, Dionisios G. and Tsapatsis, Michael and Boscoboinik, J. Anibal},
abstractNote = {Monitoring the effects of mild hydrothermal conditions, in situ, on siliceous materials remains challenging using surface science techniques, which often require electrically conductive substrates. The emergence of two-dimensional (2-D) siliceous nanomaterials deposited on metal single crystals overcomes this limitation. Here, we use infrared reflection absorption spectroscopy (IRRAS) to study the effects of mild hydrothermal conditions, in situ, on 2-D model systems, namely, all-Si MFI nanosheets supported on Au(111) and a polymorphous bilayer silicate supported on Ru(0001). We find that the formation of silanol groups (SiOH) occurs at 473 and 573 K under a H2O pressure of 3 mbar in the MFI nanosheets, but not in the polymorphous bilayer silicate. The effects of mild hydrothermal conditions are reversible in the MFI nanosheets and do not result in framework degradation. Implications shown here provide a fundamental understanding of the impact of mild hydrothermal conditions on the 2-D siliceous nanomaterials and serve as a starting point when considering these effects on three-dimensional (3-D) ones.},
doi = {10.1021/acs.jpcc.0c03875},
journal = {Journal of Physical Chemistry. C},
number = 33,
volume = 124,
place = {United States},
year = {Sun Jul 26 00:00:00 EDT 2020},
month = {Sun Jul 26 00:00:00 EDT 2020}
}
Works referenced in this record:
From Microporous to Mesoporous Molecular Sieve Materials and Their Use in Catalysis
journal, October 1997
- Corma, Avelino
- Chemical Reviews, Vol. 97, Issue 6, p. 2373-2420
Ordered porous materials for emerging applications
journal, June 2002
- Davis, Mark E.
- Nature, Vol. 417, Issue 6891, p. 813-821
Renewable p -Xylene from 2,5-Dimethylfuran and Ethylene Using Phosphorus-Containing Zeolite Catalysts
journal, January 2017
- Cho, Hong Je; Ren, Limin; Vattipalli, Vivek
- ChemCatChem, Vol. 9, Issue 3
Dispersible Exfoliated Zeolite Nanosheets and Their Application as a Selective Membrane
journal, October 2011
- Varoon, K.; Zhang, X.; Elyassi, B.
- Science, Vol. 334, Issue 6052, p. 72-75
Sorption of volatile organic compounds on hydrophobic zeolites
journal, April 2000
- Meininghaus, Carsten K. W.; Prins, Roel
- Microporous and Mesoporous Materials, Vol. 35-36
Evaluation of hybrid silica sols for stable microporous membranes using high-throughput screening
journal, April 2010
- Kreiter, R.; Rietkerk, M. D. A.; Castricum, H. L.
- Journal of Sol-Gel Science and Technology, Vol. 57, Issue 3
Long-term steam stability of MWW structure zeolites (MCM-22 and ITQ-1)
journal, July 2014
- Elyassi, Bahman; Zhang, Xueyi; Tsapatsis, Michael
- Microporous and Mesoporous Materials, Vol. 193
Steam‐Induced Coarsening of Single‐Unit‐Cell MFI Zeolite Nanosheets and Its Effect on External Surface Brønsted Acid Catalysis
journal, April 2020
- Guefrachi, Yasmine; Sharma, Geetu; Xu, Dandan
- Angewandte Chemie International Edition, Vol. 59, Issue 24
Combined solid-state NMR, FT-IR and computational studies on layered and porous materials
journal, January 2018
- Paul, Geo; Bisio, Chiara; Braschi, Ilaria
- Chemical Society Reviews, Vol. 47, Issue 15
Tutorial on Powder X-ray Diffraction for Characterizing Nanoscale Materials
journal, July 2019
- Holder, Cameron F.; Schaak, Raymond E.
- ACS Nano, Vol. 13, Issue 7
The Silica–Water Interface: How the Silanols Determine the Surface Acidity and Modulate the Water Properties
journal, February 2012
- Sulpizi, Marialore; Gaigeot, Marie-Pierre; Sprik, Michiel
- Journal of Chemical Theory and Computation, Vol. 8, Issue 3
Exploring Zeolite Chemistry with the Tools of Surface Science: Challenges, Opportunities, and Limitations
journal, September 2014
- Boscoboinik, J. Anibal; Shaikhutdinov, Shamil
- Catalysis Letters, Vol. 144, Issue 12
Modeling Zeolites with Metal-Supported Two-Dimensional Aluminosilicate Films
journal, April 2012
- Boscoboinik, Jorge Anibal; Yu, Xin; Yang, Bing
- Angewandte Chemie International Edition, Vol. 51, Issue 24
Thin silica films on Ru(0001): monolayer, bilayer and three-dimensional networks of [SiO4] tetrahedra
journal, January 2012
- Yang, Bing; Kaden, William E.; Yu, Xin
- Physical Chemistry Chemical Physics, Vol. 14, Issue 32
Support effects on the atomic structure of ultrathin silica films on metals
journal, April 2012
- Yu, Xin; Yang, Bing; Anibal Boscoboinik, Jorge
- Applied Physics Letters, Vol. 100, Issue 15
Beyond Ordered Materials: Understanding Catalytic Sites on Amorphous Solids
journal, October 2017
- Goldsmith, Bryan R.; Peters, Baron; Johnson, J. Karl
- ACS Catalysis, Vol. 7, Issue 11
Solution-processable exfoliated zeolite nanosheets purified by density gradient centrifugation
journal, May 2013
- Agrawal, Kumar Varoon; Topuz, Berna; Jiang, Zheyu
- AIChE Journal, Vol. 59, Issue 9, p. 3458-3467
Ultra-selective high-flux membranes from directly synthesized zeolite nanosheets
journal, March 2017
- Jeon, Mi Young; Kim, Donghun; Kumar, Prashant
- Nature, Vol. 543, Issue 7647
Conversion of Methanol and Glycerol into Gasoline via ZSM-5 Catalysis
journal, November 2013
- Luo, Guanqun; McDonald, Armando G.
- Energy & Fuels, Vol. 28, Issue 1
para -Xylene Ultra-selective Zeolite MFI Membranes Fabricated from Nanosheet Monolayers at the Air-Water Interface
journal, December 2017
- Kim, Donghun; Jeon, Mi Young; Stottrup, Benjamin L.
- Angewandte Chemie International Edition, Vol. 57, Issue 2
Large-Grain, Oriented, and Thin Zeolite MFI Films from Directly Synthesized Nanosheet Coatings
journal, May 2018
- Kim, Donghun; Shete, Meera; Tsapatsis, Michael
- Chemistry of Materials, Vol. 30, Issue 10
Studying two-dimensional zeolites with the tools of surface science: MFI nanosheets on Au(111)
journal, February 2017
- Kestell, John D.; Zhong, Jian-Qiang; Shete, Meera
- Catalysis Today, Vol. 280
FT-IR Evidence of Two Distinct Protonic Sites in BEA Zeolite: Consequences on Cationic Exchange and on Acido-Basic Properties in the Presence of Cesium
journal, June 2008
- Bisio, C.; Martra, G.; Coluccia, S.
- The Journal of Physical Chemistry C, Vol. 112, Issue 28
Surficial Siloxane-to-Silanol Interconversion during Room-Temperature Hydration/Dehydration of Amorphous Silica Films Observed by ATR-IR and TIR-Raman Spectroscopy
journal, February 2016
- Warring, Suzanne L.; Beattie, David A.; McQuillan, A. James
- Langmuir, Vol. 32, Issue 6
New insights in the formation of silanol defects in silicalite-1 by water intrusion under high pressure
journal, January 2010
- Karbowiak, Thomas; Saada, Mohamed-Ali; Rigolet, Séverinne
- Physical Chemistry Chemical Physics, Vol. 12, Issue 37
Steaming of Zeolite BEA and Its Effect on Acidity: A Comparative NMR and IR Spectroscopic Study
journal, April 2011
- Maier, Sarah M.; Jentys, Andreas; Lercher, Johannes A.
- The Journal of Physical Chemistry C, Vol. 115, Issue 16
The surface chemistry of amorphous silica. Zhuravlev model
journal, November 2000
- Zhuravlev, L. T.
- Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 173, Issue 1-3
Insights into Silica Bilayer Hydroxylation and Dissolution
journal, November 2016
- Kaden, William E.; Pomp, Sascha; Sterrer, Martin
- Topics in Catalysis, Vol. 60, Issue 6-7
Fast room temperature lability of aluminosilicate zeolites
journal, October 2019
- Heard, Christopher J.; Grajciar, Lukas; Rice, Cameron M.
- Nature Communications, Vol. 10, Issue 1
Hydroxylation of Metal-Supported Sheet-Like Silica Films
journal, April 2013
- Yang, B.; Emmez, E.; Kaden, W. E.
- The Journal of Physical Chemistry C, Vol. 117, Issue 16
Temperature dependence of IR absorption of OH species in clinopyroxene
journal, September 2010
- Yang, Y.; Xia, Q.; Feng, M.
- American Mineralogist, Vol. 95, Issue 10
Electron stimulated hydroxylation of a metal supported silicate film
journal, January 2016
- Yu, Xin; Emmez, Emre; Pan, Qiushi
- Physical Chemistry Chemical Physics, Vol. 18, Issue 5
Quantification of Water and Silanol Species on Various Silicas by Coupling IR Spectroscopy and in-Situ Thermogravimetry
journal, May 2009
- Gallas, Jean-Paul; Goupil, Jean-Michel; Vimont, Alexandre
- Langmuir, Vol. 25, Issue 10
Adsorption of water and 18 O exchange of surface hydroxyl groups on silica
journal, August 1970
- Morrow, B. A.; Devi, A.
- Canadian Journal of Chemistry, Vol. 48, Issue 15
Infrared studies of reactions on oxide surfaces. 7. Mechanism of the adsorption of water and ammonia on dehydroxylated silica
journal, December 1976
- Morrow, B. A.; Cody, I. A.; Lee, Lydia S. M.
- The Journal of Physical Chemistry, Vol. 80, Issue 25
Novel aspects of mid and far IR Fourier spectroscopy applied to surface and adsorption studies on SiO2
journal, September 1987
- Hoffmann, Pedro; Knözinger, Erich
- Surface Science, Vol. 188, Issue 1-2