Highly Dispersed SiO x /Al 2 O 3 Catalysts Illuminate the Reactivity of Isolated Silanol Sites

Mouat, Aidan R.; George, Cassandra; Kobayashi, Takeshi; Pruski, Marek; van Duyne, Richard P.; Marks, Tobin J.; Stair, Peter C.

doi:10.1002/ange.201505452

Title: Highly Dispersed SiO _x /Al ₂ O ₃ Catalysts Illuminate the Reactivity of Isolated Silanol Sites (in German)

Journal Article · Wed Sep 23 00:00:00 EDT 2015 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.201505452· OSTI ID:2279222

Mouat, Aidan R.; George, Cassandra; Kobayashi, Takeshi; Pruski, Marek; van Duyne, Richard P.; Marks, Tobin J.; Stair, Peter C.

Abstract The reaction of γ‐alumina with tetraethylorthosilicate (TEOS) vapor at low temperatures selectively yields monomeric SiO _x species on the alumina surface. These isolated (‐AlO) ₃ Si(OH) sites are characterized by PXRD, XPS, DRIFTS of adsorbed NH ₃ , CO, and pyridine, and ²⁹ Si and ²⁷ Al DNP‐enhanced solid‐state NMR spectroscopy. The formation of isolated sites suggests that TEOS reacts preferentially at strong Lewis acid sites on the γ‐Al ₂ O ₃ surface, functionalizing the surface with “mild” Brønsted acid sites. For liquid‐phase catalytic cyclohexanol dehydration, these SiO _x sites exhibit up to 3.5‐fold higher specific activity than the parent alumina with identical selectivity.

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Sponsoring Organization:: USDOE

OSTI ID:: 2279222

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 127 Journal Issue: 45; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: German

References (49)

A quantum-chemical approach to the generation of solid acidity in composite metal oxides Kawakami, Hiroshi; Yoshida, Satohiro; Yonezawa, Teijiro Journal of the Chemical Society, Faraday Transactions 2, Vol. 80, Issue 3 https://doi.org/10.1039/f29848000205	journal	January 1984
A Fast XPS study of the surface chemistry of ethanol over Pt{111} Lee, Adam F.; Gawthrope, David E.; Hart, Nicholas J. Surface Science, Vol. 548, Issue 1-3 https://doi.org/10.1016/j.susc.2003.11.004	journal	January 2004
Acidic Crystalline Aluminosilicates. New Superactive, Superselective Cracking Catalysts Plank, C. J.; Rosinski, E. J.; Hawthorne, W. P. Industrial & Engineering Chemistry Product Research and Development, Vol. 3, Issue 3 https://doi.org/10.1021/i360011a001	journal	September 1964
Thin silica layer on alumina: evidence of the acidity in the monolayer Niwa, Miki.; Katada, Naonobu.; Murakami, Yuichi. The Journal of Physical Chemistry, Vol. 94, Issue 16 https://doi.org/10.1021/j100379a052	journal	August 1990
The Acidity of Zeolites: Concepts, Measurements and Relation to Catalysis: A Review on Experimental and Theoretical Methods for the Study of Zeolite Acidity Derouane, E. G.; Védrine, J. C.; Pinto, R. Ramos Catalysis Reviews, Vol. 55, Issue 4 https://doi.org/10.1080/01614940.2013.822266	journal	October 2013
Acidic catalysts for the dehydration of glycerol: Activity and deactivation Suprun, Wladimir; Lutecki, Michal; Haber, Thomas Journal of Molecular Catalysis A: Chemical, Vol. 309, Issue 1-2 https://doi.org/10.1016/j.molcata.2009.04.017	journal	August 2009
Solid Acids and Bases Tanabe, Kozo Solid Acids and Bases: Their Catalytic Properties https://doi.org/10.1016/B978-0-12-683250-1.50005-5	book	January 1970
XPS analysis of oxides Paparazzo, E. Surface and Interface Analysis, Vol. 12, Issue 2 https://doi.org/10.1002/sia.740120210	journal	July 1988
SURFACE HYDROXYL GROUPS ON γ-ALUMINA ¹ Peri, J. B.; Hannan, R. B. The Journal of Physical Chemistry, Vol. 64, Issue 10 https://doi.org/10.1021/j100839a044	journal	October 1960
Adsorption Assisted Desorption of NH ₃ on γ-Alumina Studied with Positron Emission Profiling Sobczyk, D. P.; Hesen, J. J. G.; van Grondelle, J. Catalysis Letters, Vol. 94, Issue 1/2 https://doi.org/10.1023/B:CATL.0000019328.16620.1d	journal	April 2004
Catalytic dehydration of ethanol over silica-alumina Roca, F. Journal of Catalysis, Vol. 14, Issue 2 https://doi.org/10.1016/0021-9517(69)90414-X	journal	June 1969
FT-IR characterization of silicated aluminas, active olefin skeletal isomerization catalysts Finocchio, Elisabetta; Busca, Guido; Rossini, Stefano Catalysis Today, Vol. 33, Issue 1-3 https://doi.org/10.1016/S0920-5861(96)00106-X	journal	January 1997
Deactivation of a silica-alumina catalyst by coke deposition Garcia-Ochoa, Felix; Santos, Aurora Industrial & Engineering Chemistry Research, Vol. 32, Issue 11 https://doi.org/10.1021/ie00023a028	journal	November 1993
Modification of polymer-gel structures Yoldas, Bulent E. Journal of Non-Crystalline Solids, Vol. 63, Issue 1-2 https://doi.org/10.1016/0022-3093(84)90393-4	journal	February 1984
Synthesis of amorphous aluminosilicates by grafting: Tuning the building and final structure of the deposit by selecting the appropriate synthesis conditions Caillot, Maxime; Chaumonnot, Alexandra; Digne, Mathieu Microporous and Mesoporous Materials, Vol. 185 https://doi.org/10.1016/j.micromeso.2013.10.032	journal	February 2014
Surface chemistry of atomic layer deposition: A case study for the trimethylaluminum/water process Puurunen, Riikka L. Journal of Applied Physics, Vol. 97, Issue 12, Article No. 121301 https://doi.org/10.1063/1.1940727	journal	June 2005
Impact of solvent for individual steps of phenol hydrodeoxygenation with Pd/C and HZSM-5 as catalysts He, Jiayue; Zhao, Chen; Lercher, Johannes A. Journal of Catalysis, Vol. 309 https://doi.org/10.1016/j.jcat.2013.09.009	journal	January 2014
FT-IR Studies on Light Olefin Skeletal Isomerization Catalysis Trombetta, Marcella; Busca, Guido; Rossini, Stefano Journal of Catalysis, Vol. 179, Issue 2 https://doi.org/10.1006/jcat.1998.2251	journal	October 1998
The surface of transitional aluminas: A critical review Busca, Guido Catalysis Today, Vol. 226 https://doi.org/10.1016/j.cattod.2013.08.003	journal	May 2014
2,6-Dimethylpyridine as a probe of the strength of Brønsted acid sites: study on zeolites. Application to alumina Oliviero, Laetitia; Vimont, Alexandre; Lavalley, Jean-Claude Phys. Chem. Chem. Phys., Vol. 7, Issue 8 https://doi.org/10.1039/B500689A	journal	January 2005
Catalytically Active Sites for the Beckmann Rearrangement of Cyclohexanone Oxime to ε-Caprolactam Heitmann, G. P.; Dahlhoff, G.; Hölderich, W. F. Journal of Catalysis, Vol. 186, Issue 1 https://doi.org/10.1006/jcat.1999.2552	journal	August 1999
Quantification of Brønsted Acid Sites of Grafted Amorphous Silica-Alumina Compounds and their Turnover Frequency in m -Xylene Isomerization Caillot, Maxime; Chaumonnot, Alexandra; Digne, Mathieu ChemCatChem, Vol. 5, Issue 12 https://doi.org/10.1002/cctc.201300560	journal	October 2013
Grafted Poly(1→4-β-glucan) Strands on Silica: A Comparative Study of Surface Reactivity as a Function of Grafting Density Gazit, Oz M.; Katz, Alexander Langmuir, Vol. 28, Issue 1 https://doi.org/10.1021/la2036482	journal	December 2011
Understanding the Role of Defect Sites in Glucan Hydrolysis on Surfaces Gazit, Oz M.; Katz, Alexander Journal of the American Chemical Society, Vol. 135, Issue 11 https://doi.org/10.1021/ja311918z	journal	March 2013
Dynamic nuclear polarization at high magnetic fields Maly, Thorsten; Debelouchina, Galia T.; Bajaj, Vikram S. The Journal of Chemical Physics, Vol. 128, Issue 5 https://doi.org/10.1063/1.2833582	journal	February 2008
Surface Modification of Au/TiO ₂ Catalysts by SiO ₂ via Atomic Layer Deposition Ma, Zhen; Brown, Suree; Howe, Jane Y. The Journal of Physical Chemistry C, Vol. 112, Issue 25 https://doi.org/10.1021/jp801484h	journal	May 2008
The variety of Brønsted acid sites in amorphous aluminosilicates and zeolites Caillot, Maxime; Chaumonnot, Alexandra; Digne, Mathieu Journal of Catalysis, Vol. 316 https://doi.org/10.1016/j.jcat.2014.05.002	journal	July 2014
Microstructure of silica monolayer solid acid catalysts determined by 29Si NMR spectroscopy Katada, Naonobu; Niwa, Miki Research on Chemical Intermediates, Vol. 24, Issue 5 https://doi.org/10.1163/156856798X00014	journal	May 1998
A Novel Method To Synthesize Amorphous Silica−Alumina Materials with Mesoporous Distribution without Using Templates and Pore-Regulating Agents Yao, Nan; Xiong, Guoxing; He, Mingyuan Chemistry of Materials, Vol. 14, Issue 1 https://doi.org/10.1021/cm010270w	journal	January 2002
Surface Enhanced NMR Spectroscopy by Dynamic Nuclear Polarization Lesage, Anne; Lelli, Moreno; Gajan, David Journal of the American Chemical Society, Vol. 132, Issue 44 https://doi.org/10.1021/ja104771z	journal	November 2010
Mechanisms of xylene isomerization over acidic solid catalysts Guisnet, M.; Gnep, N. S.; Morin, S. Microporous and Mesoporous Materials, Vol. 35-36 https://doi.org/10.1016/S1387-1811(99)00207-3	journal	April 2000
Brønsted acid sites of zeolitic strength in amorphous silica-alumina Poduval, Dilip G.; van Veen, J. A. Rob; Rigutto, Marcello S. Chemical Communications, Vol. 46, Issue 20 https://doi.org/10.1039/c000019a	journal	January 2010
Catalytic conversion of methane to more useful chemicals and fuels: a challenge for the 21st century Lunsford, Jack H. Catalysis Today, Vol. 63, Issue 2-4, p. 165-174 https://doi.org/10.1016/S0920-5861(00)00456-9	journal	December 2000
Catalytic Properties of Silica-Alumina Prepared by Chemical Vapor Deposition Sato, Satoshi; Toita, Masato; Yu, Yu-Qing Chemistry Letters, Vol. 16, Issue 8 https://doi.org/10.1246/cl.1987.1535	journal	August 1987
Synthesis of ketenes from carboxylic acids on functionalized silica monoliths at short contact times Martinez, R.; Huff, M. C.; Barteau, M. A. Applied Catalysis A: General, Vol. 200, Issue 1-2 https://doi.org/10.1016/S0926-860X(00)00649-9	journal	August 2000
A methanol to olefins review: Diffusion, coke formation and deactivation on SAPO type catalysts Chen, D.; Moljord, K.; Holmen, A. Microporous and Mesoporous Materials, Vol. 164 https://doi.org/10.1016/j.micromeso.2012.06.046	journal	December 2012
Model silica-alumina acid catalysts for surface science and catalysis studies prepared by argon ion beam sputter deposition using HY-zeolite targets B�sz�rm�nyi, Istvan; Nakayama, Taisei; McIntyre, Brian Catalysis Letters, Vol. 10, Issue 5-6 https://doi.org/10.1007/BF00769169	journal	January 1991
ALD of SiO[sub 2] at Room Temperature Using TEOS and H[sub 2]O with NH[sub 3] as the Catalyst Ferguson, J. D.; Smith, E. R.; Weimer, A. W. Journal of The Electrochemical Society, Vol. 151, Issue 8 https://doi.org/10.1149/1.1768548	journal	January 2004
X-ray photoelectron spectroscopy of low-temperature anodic silicon oxides: LOW-TEMPERATURE ANODIC SILICON OXIDES Galán, L.; Montero, I.; Rueda, F. Surface and Interface Analysis, Vol. 19, Issue 1-12 https://doi.org/10.1002/sia.740190189	journal	June 1992
Fine control of the pore-opening size of the zeolite mordenite by chemical vapour deposition of silicon alkoxide Niwa, Miki; Kato, Satoshi; Hattori, Tadashi Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 80, Issue 11 https://doi.org/10.1039/f19848003135	journal	January 1984
Infrared spectrum of ammonia adsorbed on silica-alumina Basila, Michael R.; Kantner, Theodore R. The Journal of Physical Chemistry, Vol. 71, Issue 3 https://doi.org/10.1021/j100862a001	journal	February 1967
Characterization of oxide surfaces and zeolites by carbon monoxide as an IR probe molecule Hadjiivanov, Konstantin I.; Vayssilov, Georgi N. Advances in Catalysis https://doi.org/10.1016/S0360-0564(02)47008-3	book	January 2002
Structure of SiO2 and Al2O3 Monolayer Catalysts: Investigation by Infrared-Spectroscopy and 29Si MAS NMR Sheng, T. C.; Lang, S.; Morrow, B. A. Journal of Catalysis, Vol. 148, Issue 1 https://doi.org/10.1006/jcat.1994.1215	journal	July 1994
Experimental and QM/MM investigation of the hydrated silica surface reactivity Casarin, Maurizio; Falcomer, Daniele; Glisenti, Antonella Chemical Physics Letters, Vol. 405, Issue 4-6 https://doi.org/10.1016/j.cplett.2005.02.076	journal	April 2005
A 29Si NMR investigation of the structure of amorphous silica—alumina supports McMillan, M.; Brinen, J. S.; Carruthers, J. D. Colloids and Surfaces, Vol. 38, Issue 1 https://doi.org/10.1016/0166-6622(89)80150-7	journal	January 1989
Viscous flow reactor with quartz crystal microbalance for thin film growth by atomic layer deposition Elam, J. W.; Groner, M. D.; George, S. M. Review of Scientific Instruments, Vol. 73, Issue 8, p. 2981-2987 https://doi.org/10.1063/1.1490410	journal	August 2002
Atomic layer deposition of SiO2 at room temperature using NH3-catalyzed sequential surface reactions Klaus, J. W.; George, S. M. Surface Science, Vol. 447, Issue 1-3 https://doi.org/10.1016/S0039-6028(99)01119-X	journal	February 2000
Chemistry of Cracking Catalysts Thomas, Charles L. Industrial & Engineering Chemistry, Vol. 41, Issue 11 https://doi.org/10.1021/ie50479a042	journal	November 1949
The nature of the relative bonding chemistry in zeolites: An XPS study Barr, Tery L. Zeolites, Vol. 10, Issue 8 https://doi.org/10.1016/0144-2449(90)90058-Y	journal	November 1990

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