Controlled Generation of TiOx–Au Interface Using Titanium Molecular Complex Bearing Pyridyl Anchors: Synthesis, Characterization and Catalysis

Wang, Zhen; Hou, Xianliang; Wu, Yi Y.; Shen, Jingmei; Li, Tiehu; Fang, Changqing; Kung, Mayfair C.; Kung, Harold H.

doi:10.1007/s11244-018-0941-2

Controlled Generation of TiO_x–Au Interface Using Titanium Molecular Complex Bearing Pyridyl Anchors: Synthesis, Characterization and Catalysis

Journal Article · Tue Jun 12 00:00:00 EDT 2018 · Topics in Catalysis

DOI:https://doi.org/10.1007/s11244-018-0941-2· OSTI ID:1870990

Wang, Zhen ^[1]; Hou, Xianliang ^[2]; Wu, Yi Y. ^[3]; Shen, Jingmei ^[3]; Li, Tiehu ^[2]; Fang, Changqing ^[4]; Kung, Mayfair C. ^[3]; Kung, Harold H. ^[3]

Xi'an Univ. of Technology, Xi'an, Shaanxi (China); Northwestern Univ., Evanston, IL (United States); Northwestern University
Northwestern Polytechnical Univ., Xi'an, Shaanxi (China)
Northwestern Univ., Evanston, IL (United States)
Xi'an Univ. of Technology, Xi'an, Shaanxi (China)

Interfacial perimeter sites between metal and support are often important for catalysis. A mononuclear titanium siloxy complex III, Ti(acac)₂[OSiC₆H₅N(OCH₃)₂]₂ was synthesized to generate TiOx units of different degrees of clustering to decorate Au nanoparticles. Two different methods of preparation were examined; one was to deposit III onto Au/SiO₂ and the other was to form III-covered Au nanoparticle first before deposition onto SiO₂. The former method generated more highly dispersed TiO_x units, while larger domains of TiO₂ were formed with the latter method, as deduced by UV–vis and XAS characterization. A model was proposed to explain how TiO_x dispersity could be related to the preparative procedures. These samples were further tested as catalysts in selective oxidation of propane in a stream of O₂ and H₂. They exhibited different product selectivities. The sample with more dispersed TiO_x units were more selective for acetone formation versus propene formation. The results confirmed the important role of both the Au–TiO_x interface at the perimeter and the extent of Ti isolation in the TiO_x phase in the reaction.

View Accepted Manuscript (DOE)

Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: China Scholarship Council (CSC); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-03ER15457

OSTI ID:: 1870990

Alternate ID(s):: OSTI ID: 1459020

Journal Information:: Topics in Catalysis, Journal Name: Topics in Catalysis Journal Issue: 9-11 Vol. 61; ISSN 1022-5528

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

References (42)

The Usefulness of Time-Dependent Density Functional Theory to Describe the Electronic Spectra of Ti-Containing Catalysts de la Peña O'Shea, Victor. A.; Capel-Sanchez, Maricarmen; Blanco-Brieva, Gema Angewandte Chemie International Edition, Vol. 42, Issue 47 https://doi.org/10.1002/anie.200351452	journal	December 2003
Effect of Local Structure on the UV-Visible Absorption Edges of Molybdenum Oxide Clusters and Supported Molybdenum Oxides Weber, R. S. Journal of Catalysis, Vol. 151, Issue 2 https://doi.org/10.1006/jcat.1995.1052	journal	February 1995
Synthesis, Characterization, and Catalytic Activity of Ti-MCM-41 Structures Blasco, T.; Corma, A.; Navarro, M. T. Journal of Catalysis, Vol. 156, Issue 1 https://doi.org/10.1006/jcat.1995.1232	journal	September 1995
Amorphous Microporous Titania–Silica Mixed Oxides: Preparation, Characterization, and Catalytic Redox Properties Klein, S.; Thorimbert, S.; Maier, W. F. Journal of Catalysis, Vol. 163, Issue 2 https://doi.org/10.1006/jcat.1996.0349	journal	October 1996
Gold-catalysed oxidation of carbon monoxide Bond, Geoffrey C.; Thompson, David T. Gold Bulletin, Vol. 33, Issue 2 https://doi.org/10.1007/BF03216579	journal	June 2000
Tailored Oxide Materials via Thermolytic Molecular Precursor (TMP) Methods Fujdala, Kyle L.; Brutchey, Richard L.; Tilley, T. Don Surface and Interfacial Organometallic Chemistry and Catalysis https://doi.org/10.1007/b138074	book	January 2005
Understanding the effect of halide poisoning in CO oxidation over Au/TiO2 Oxford, S. M.; Henao, J. D.; Yang, J. H. Applied Catalysis A: General, Vol. 339, Issue 2 https://doi.org/10.1016/j.apcata.2008.01.025	journal	May 2008
Selective oxidation of hydrocarbons on supported Au catalysts Mashayekhi, Neema A.; Kung, Mayfair C.; Kung, Harold H. Catalysis Today, Vol. 238 https://doi.org/10.1016/j.cattod.2013.12.055	journal	December 2014
The effect of gold particle size on AuAu bond length and reactivity toward oxygen in supported catalysts Miller, J. T.; Kropf, A. J.; Zha, Y. Journal of Catalysis, Vol. 240, Issue 2 https://doi.org/10.1016/j.jcat.2006.04.004	journal	June 2006
Mechanistic study of propane selective oxidation with H2 and O2 on Au/TS-1 Bravosuarez, J.; Bando, K.; Fujitani, T. Journal of Catalysis, Vol. 257, Issue 1 https://doi.org/10.1016/j.jcat.2008.04.004	journal	July 2008
Quantifying accessible sites and reactivity on titania–silica (photo)catalysts: Refining TOF calculations Eaton, Todd R.; Campos, Michael P.; Gray, Kimberly A. Journal of Catalysis, Vol. 309 https://doi.org/10.1016/j.jcat.2013.09.015	journal	January 2014
Efficient Ceria–Platinum Inverse Catalyst for Partial Oxidation of Methanol Ostroverkh, Anna; Johánek, Viktor; Kúš, Peter Langmuir, Vol. 32, Issue 25 https://doi.org/10.1021/acs.langmuir.6b01316	journal	June 2016
Direct Visualization of Catalytically Active Sites at the FeO–Pt(111) Interface Kudernatsch, Wilhelmine; Peng, Guowen; Zeuthen, Helene ACS Nano, Vol. 9, Issue 8 https://doi.org/10.1021/acsnano.5b02339	journal	June 2015
Unique Properties of Ceria Nanoparticles Supported on Metals: Novel Inverse Ceria/Copper Catalysts for CO Oxidation and the Water-Gas Shift Reaction Senanayake, Sanjaya D.; Stacchiola, Dario; Rodriguez, Jose A. Accounts of Chemical Research, Vol. 46, Issue 8 https://doi.org/10.1021/ar300231p	journal	January 2013
New Vanadium Tris( tert -butoxy)siloxy Complexes and Their Thermolytic Conversions to Vanadia−Silica Materials Fujdala, Kyle L.; Tilley, T. Don Chemistry of Materials, Vol. 14, Issue 3 https://doi.org/10.1021/cm011524g	journal	March 2002
The state of Ti in titanoaluminosilicates isomorphous with zeolite .beta. Blasco, T.; Camblor, M. A.; Corma, A. Journal of the American Chemical Society, Vol. 115, Issue 25 https://doi.org/10.1021/ja00078a020	journal	December 1993
Supported Gold Nanoparticles from Quantum Dot to Mesoscopic Size Scale: Effect of Electronic and Structural Properties on Catalytic Hydrogenation of Conjugated Functional Groups Claus, Peter; Brückner, Angelika; Mohr, Christian Journal of the American Chemical Society, Vol. 122, Issue 46 https://doi.org/10.1021/ja0012974	journal	November 2000
Silica-Supported, Single-Site Titanium Catalysts for Olefin Epoxidation. A Molecular Precursor Strategy for Control of Catalyst Structure Jarupatrakorn, Jonggol; Tilley, T. Don Journal of the American Chemical Society, Vol. 124, Issue 28 https://doi.org/10.1021/ja0202208	journal	July 2002
Structural Assessment and Catalytic Consequences of the Oxygen Coordination Environment in Grafted Ti−Calixarenes Notestein, Justin M.; Andrini, Leandro R.; Kalchenko, Vitaly I. Journal of the American Chemical Society, Vol. 129, Issue 5 https://doi.org/10.1021/ja065830c	journal	February 2007
Nature of Electron Transport by Pyridine-Based Tripodal Anchors: Potential for Robust and Conductive Single-Molecule Junctions with Gold Electrodes Ie, Yutaka; Hirose, Tomoya; Nakamura, Hisao Journal of the American Chemical Society, Vol. 133, Issue 9 https://doi.org/10.1021/ja109577f	journal	March 2011
Solvent and Ligand Effects on the Localized Surface Plasmon Resonance (LSPR) of Gold Colloids Ghosh, Sujit Kumar; Nath, Sudip; Kundu, Subrata The Journal of Physical Chemistry B, Vol. 108, Issue 37 https://doi.org/10.1021/jp047021q	journal	September 2004
In Situ Transient FTIR and XANES Studies of the Evolution of Surface Species in CO Oxidation on Au/TiO ₂ Henao, Juan D.; Caputo, Tiziana; Yang, Jeff H. The Journal of Physical Chemistry B, Vol. 110, Issue 17 https://doi.org/10.1021/jp0568733	journal	May 2006
Structural Investigation of Au Catalysts on TiO ₂ −SiO ₂ Supports: Nature of the Local Structure of Ti and Au Atoms by EXAFS and XANES Schwartz, Viviane; Mullins, David R.; Yan, Wenfu The Journal of Physical Chemistry C, Vol. 111, Issue 46 https://doi.org/10.1021/jp074426c	journal	October 2007
UV−Visible Diffuse Reflectance Spectroscopy of Zeolite-Hosted Mononuclear Titanium Oxide Species Klaas, Joachim; Schulz-Ekloff, Günter; Jaeger, Nils I. The Journal of Physical Chemistry B, Vol. 101, Issue 8 https://doi.org/10.1021/jp9627133	journal	February 1997
Optical Absorption Spectra of Nanocrystal Gold Molecules Alvarez, Marcos M.; Khoury, Joseph T.; Schaaff, T. Gregory The Journal of Physical Chemistry B, Vol. 101, Issue 19 https://doi.org/10.1021/jp962922n	journal	May 1997
Size and Temperature Dependence of the Plasmon Absorption of Colloidal Gold Nanoparticles Link, Stephan; El-Sayed, Mostafa A. The Journal of Physical Chemistry B, Vol. 103, Issue 21 https://doi.org/10.1021/jp984796o	journal	May 1999
Effect of the Solution Refractive Index on the Color of Gold Colloids Underwood, Sylvia; Mulvaney, Paul Langmuir, Vol. 10, Issue 10 https://doi.org/10.1021/la00022a011	journal	October 1994
Synthesis and Characterization of Titania Prepared by Using a Photoassisted Sol−Gel Method Liu, Haimei; Yang, Wensheng; Ma, Ying Langmuir, Vol. 19, Issue 7 https://doi.org/10.1021/la026600o	journal	April 2003
Bis(pyridyl)siloxane Oligomeric Ligands for Palladium(II) Acetate: Synthesis and Binding Properties Missaghi, Michael N.; Galloway, John M.; Kung, Harold H. Organometallics, Vol. 29, Issue 17 https://doi.org/10.1021/om100316n	journal	September 2010
Selective oxidation with dioxygen by gold nanoparticle catalysts derived from 55-atom clusters Turner, Mark; Golovko, Vladimir B.; Vaughan, Owain P. H. Nature, Vol. 454, Issue 7207 https://doi.org/10.1038/nature07194	journal	August 2008
Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity Corma, Avelino; Concepción, Patricia; Boronat, Mercedes Nature Chemistry, Vol. 5, Issue 9 https://doi.org/10.1038/nchem.1721	journal	August 2013
Controlling activity and selectivity using water in the Au-catalysed preferential oxidation of CO in H2 Saavedra, Johnny; Whittaker, Todd; Chen, Zhifeng Nature Chemistry, Vol. 8, Issue 6 https://doi.org/10.1038/nchem.2494	journal	April 2016
CO bond cleavage on supported nano-gold during low temperature oxidation Carley, Albert F.; Morgan, David J.; Song, Nianxue Phys. Chem. Chem. Phys., Vol. 13, Issue 7 https://doi.org/10.1039/C0CP01852J	journal	January 2011
Amine-functionalized siloxane oligomer facilitated synthesis of subnanometer colloidal Au particles Wang, Zhen; Beletskiy, Evgeny V.; Lee, Sungsik Journal of Materials Chemistry A, Vol. 3, Issue 4 https://doi.org/10.1039/C4TA05954A	journal	January 2015
Ga[OSi(O ^t Bu) ₃ ] ₃ ·THF, a thermolytic molecular precursor for high surface area gallium-containing silica materials of controlled dispersion and stoichiometry Dombrowski, James P.; Johnson, Gregory R.; Bell, Alexis T. Dalton Transactions, Vol. 45, Issue 27 https://doi.org/10.1039/C6DT01676F	journal	January 2016
Metal nanoparticle catalysts decorated with metal oxide clusters Mashayekhi, Neema A.; Wu, Yi Y.; Kung, Mayfair C. Chemical Communications, Vol. 48, Issue 81 https://doi.org/10.1039/c2cc34885c	journal	January 2012
Au–metal oxide support interface as catalytic active sites Wu, Yi Y.; Mashayekhi, Neema A.; Kung, Harold H. Catalysis Science & Technology, Vol. 3, Issue 11 https://doi.org/10.1039/c3cy00243h	journal	January 2013
Ti and O K edges for titanium oxides by multiple scattering calculations: Comparison to XAS and EELS spectra Wu, Z. Y.; Ouvrard, G.; Gressier, P. Physical Review B, Vol. 55, Issue 16 https://doi.org/10.1103/PhysRevB.55.10382	journal	April 1997
Ti K -edge XANES studies of Ti coordination and disorder in oxide compounds: Comparison between theory and experiment Farges, François; Brown, Gordon E.; Rehr, J. J. Physical Review B, Vol. 56, Issue 4 https://doi.org/10.1103/PhysRevB.56.1809	journal	July 1997
Determination of Ti coordination from pre-edge peaks in Ti K -edge XANES Jiang, N.; Su, D.; Spence, J. C. H. Physical Review B, Vol. 76, Issue 21 https://doi.org/10.1103/PhysRevB.76.214117	journal	December 2007
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT Ravel, B.; Newville, M. Journal of Synchrotron Radiation, Vol. 12, Issue 4 https://doi.org/10.1107/S0909049505012719	journal	June 2005
The critical role of water at the gold-titania interface in catalytic CO oxidation Saavedra, J.; Doan, H. A.; Pursell, C. J. Science, Vol. 345, Issue 6204 https://doi.org/10.1126/science.1256018	journal	September 2014

Similar Records

Probing properties of the interfacial perimeter sites in TiO_x/Au/SiO₂ with 2-propanol decomposition

Journal Article · Thu Jun 22 20:00:00 EDT 2017 · Applied Catalysis. A, General · OSTI ID:1870998

Partial PdAu nanoparticle embedding into TiO ₂ support accentuates catalytic contributions from the Au/TiO ₂ interface

Journal Article · Wed Jan 08 19:00:00 EST 2025 · Proceedings of the National Academy of Sciences of the United States of America · OSTI ID:2497867

Modification of Au/TiO(2) Nanosystems by SiO(2) Monolayers: Toward the Control of the Catalyst Activity and Stability

Journal Article · Thu Dec 31 23:00:00 EST 2009 · Journal of Physical Chemistry C · OSTI ID:1044705

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
TiOx
interface
inverse catalyst
propane oxidation
supported gold
titanium complex precursors

Controlled Generation of TiOx–Au Interface Using Titanium Molecular Complex Bearing Pyridyl Anchors: Synthesis, Characterization and Catalysis

Citation Formats

References (42)

Similar Records

Related Subjects

Controlled Generation of TiO_x–Au Interface Using Titanium Molecular Complex Bearing Pyridyl Anchors: Synthesis, Characterization and Catalysis