Quantitative Analysis of HAADF–STEM Images of MoVTeTaO M1 Phase Catalyst for Propane Ammoxidation to Acrylonitrile

Woo, Jungwon; Borisevich, Albina; Koch, Christoph; Guliants, Vadim V.

doi:10.1002/cctc.201500402

Quantitative Analysis of HAADF–STEM Images of MoVTeTaO M1 Phase Catalyst for Propane Ammoxidation to Acrylonitrile

Journal Article · Thu Jul 16 00:00:00 EDT 2015 · ChemCatChem

DOI:https://doi.org/10.1002/cctc.201500402· OSTI ID:1786155

Woo, Jungwon ^[1]; Borisevich, Albina ^[2]; Koch, Christoph ^[3]; Guliants, Vadim V. ^[1]

Department of Biomedical, Chemical, and Environmental Engineering University of Cincinnati Cincinnati OH 45221‐0012 USA
Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA
Institute for Experimental Physics Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany

Abstract

High‐angle annular dark‐field scanning transmission electron microscopy (HAADF–STEM) image simulations were performed to determine accurate metal distributions in the MoVTeTaO M1 phase catalyst for propane ammoxidation. QSTEM simulation, based on a multislice method with the frozen phonon approximation, was chosen because of the excellent agreement between experimental and simulated HAADF–STEM images. This simulation method successfully provided accurate metal distributions in the MoVTeTaO M1 phase and indicated significantly lower V occupancies of the linking sites 1, 2, 3, 4, and 7, and higher Ta occupancy in site 9 than the previously reported metal occupancies. This novel methodology for accurate HAADF–STEM image analysis is a valuable tool for accurate analysis of local chemical compositions in a wide range of ordered catalytic materials.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FG02-04ER15604

OSTI ID:: 1786155

Journal Information:: ChemCatChem, Journal Name: ChemCatChem Journal Issue: 22 Vol. 7; ISSN 1867-3880

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

Country of Publication:: Germany

Language:: English

References (48)

Direct Imaging of the MoVTeNbO M1 Phase Using An Aberration-Corrected High-Resolution Scanning Transmission Electron Microscope Pyrz, William D.; Blom, Douglas A.; Vogt, Thomas Angewandte Chemie, Vol. 120, Issue 15 https://doi.org/10.1002/ange.200705700	journal	March 2008
Direct Observation of Surface Reconstruction and Termination on a Complex Metal Oxide Catalyst by Electron Microscopy Zhu, Yihan; Wang, Qingxiao; Zhao, Lan Angewandte Chemie, Vol. 124, Issue 17 https://doi.org/10.1002/ange.201108532	journal	March 2012
Direct Imaging of the MoVTeNbO M1 Phase Using An Aberration-Corrected High-Resolution Scanning Transmission Electron Microscope Pyrz, William D.; Blom, Douglas A.; Vogt, Thomas Angewandte Chemie International Edition, Vol. 47, Issue 15 https://doi.org/10.1002/anie.200705700	journal	March 2008
Direct Observation of Surface Reconstruction and Termination on a Complex Metal Oxide Catalyst by Electron Microscopy Zhu, Yihan; Wang, Qingxiao; Zhao, Lan Angewandte Chemie International Edition, Vol. 51, Issue 17 https://doi.org/10.1002/anie.201108532	journal	March 2012
STEM HAADF Image Simulation of the Orthorhombic M1 Phase in the Mo-V-Nb-Te-O Propane Oxidation Catalyst Blom, Douglas A.; Li, Xin; Mitra, Sonali ChemCatChem, Vol. 3, Issue 6 https://doi.org/10.1002/cctc.201100049	journal	June 2011
Comparison of MoVTaTeO and MoVNbTeO M1 crystal chemistry DeSanto, P.; Buttrey, D. J.; Grasselli, R. K. Topics in Catalysis, Vol. 38, Issue 1-3 https://doi.org/10.1007/s11244-006-0068-8	journal	July 2006
Towards an Understanding of the Reaction Pathways in Propane Ammoxidation Based on the Distribution of Elements at the Active Centers of the M1 Phase of the MoV(Nb,Ta)TeO System Grasselli, R. K.; Lugmair, C. G.; Volpe, A. F. Topics in Catalysis, Vol. 54, Issue 10-12 https://doi.org/10.1007/s11244-011-9681-2	journal	May 2011
Catalytic Consequences of a Revised Distribution of Key Elements at the Active Centers of the M1 Phase of the MoVNbTeOx System Grasselli, Robert K.; Volpe, Anthony F. Topics in Catalysis, Vol. 57, Issue 14-16 https://doi.org/10.1007/s11244-014-0286-4	journal	August 2014
Simulation of annular dark field stem images using a modified multislice method Kirkland, Earl J.; Loane, Russell F.; Silcox, John Ultramicroscopy, Vol. 23, Issue 1, p. 77-96 https://doi.org/10.1016/0304-3991(87)90229-4	journal	January 1987
Simulating high-angle annular dark-field stem images including inelastic thermal diffuse scattering Wang, Z. L.; Cowley, J. M. Ultramicroscopy, Vol. 31, Issue 4 https://doi.org/10.1016/0304-3991(89)90340-9	journal	December 1989
Dynamic theory of high-angle annular-dark-field stem lattice images for a Ge/Si interface Wang, Z. L.; Cowley, J. M. Ultramicroscopy, Vol. 32, Issue 3 https://doi.org/10.1016/0304-3991(90)90005-7	journal	March 1990
Energy-filtered convergent-beam electron diffraction in STEM Xu, Peirong; Loane, Russell F.; Silcox, John Ultramicroscopy, Vol. 38, Issue 2 https://doi.org/10.1016/0304-3991(91)90113-K	journal	November 1991
Incoherent imaging of zone axis crystals with ADF STEM Loane, Russell F.; Xu, Peirong; Silcox, John Ultramicroscopy, Vol. 40, Issue 2 https://doi.org/10.1016/0304-3991(92)90054-N	journal	February 1992
Thickness effects in ADF STEM zone axis images Hillyard, Sean; Silcox, John Ultramicroscopy, Vol. 52, Issue 3-4 https://doi.org/10.1016/0304-3991(93)90043-W	journal	December 1993
Imaging elastic strains in high-angle annular dark field scanning transmission electron microscopy Perovic, D. D.; Rossouw, C. J.; Howie, A. Ultramicroscopy, Vol. 52, Issue 3-4 https://doi.org/10.1016/0304-3991(93)90046-Z	journal	December 1993
Annular dark-field imaging: Resolution and thickness effects Hillyard, Sean; Loane, Russell F.; Silcox, John Ultramicroscopy, Vol. 49, Issue 1-4 https://doi.org/10.1016/0304-3991(93)90209-G	journal	February 1993
Detector geometry, thermal diffuse scattering and strain effects in ADF STEM imaging Hillyard, Sean; Silcox, John Ultramicroscopy, Vol. 58, Issue 1 https://doi.org/10.1016/0304-3991(94)00173-K	journal	April 1995
Simulation of thermal diffuse scattering including a detailed phonon dispersion curve A. Muller, David; Edwards, Byard; J. Kirkland, Earl Ultramicroscopy, Vol. 86, Issue 3-4 https://doi.org/10.1016/S0304-3991(00)00128-5	journal	February 2001
Lattice-resolution contrast from a focused coherent electron probe. Part I Allen, L. J.; Findlay, S. D.; Oxley, M. P. Ultramicroscopy, Vol. 96, Issue 1 https://doi.org/10.1016/S0304-3991(02)00380-7	journal	July 2003
Scattering of Å-scale electron probes in silicon Dwyer, C.; Etheridge, J. Ultramicroscopy, Vol. 96, Issue 3-4 https://doi.org/10.1016/S0304-3991(03)00100-1	journal	September 2003
Incoherent imaging using dynamically scattered coherent electrons Nellist, P. D.; Pennycook, S. J. Ultramicroscopy, Vol. 78, Issue 1-4, p. 111-124 https://doi.org/10.1016/S0304-3991(99)00017-0	journal	June 1999
Thermal diffuse scattering in sub-angstrom quantitative electron microscopy—phenomenon, effects and approaches Wang, Zhong Lin Micron, Vol. 34, Issue 3-5 https://doi.org/10.1016/S0968-4328(03)00024-6	journal	April 2003
Recent developments in catalysis using nanostructured materials Shiju, N. Raveendran; Guliants, Vadim V. Applied Catalysis A: General, Vol. 356, Issue 1 https://doi.org/10.1016/j.apcata.2008.11.034	journal	March 2009
A combined HAADF STEM and density functional theory study of tantalum and niobium locations in the Mo–V–Te–Ta(Nb)–O M1 phases Yu, Junjun; Woo, Jungwon; Borisevich, Albina Catalysis Communications, Vol. 29 https://doi.org/10.1016/j.catcom.2012.09.020	journal	December 2012
Active centers in Mo–V–Nb–Te–O (amm)oxidation catalysts Grasselli, Robert K.; Buttrey, Douglas J.; DeSanto, Peter Catalysis Today, Vol. 91-92 https://doi.org/10.1016/j.cattod.2004.03.060	journal	July 2004
The effect of Nb or Ta substitution into the M1 phase of the MoV(Nb,Ta)TeO selective oxidation catalyst Pyrz, William D.; Blom, Douglas A.; Shiju, N. Raveendran Catalysis Today, Vol. 142, Issue 3-4 https://doi.org/10.1016/j.cattod.2008.10.051	journal	April 2009
Quantitative high-resolution HAADF–STEM analysis of inversion boundaries in Sb2O3-doped zinc oxide Yamazaki, T.; Nakanishi, N.; Rečnik, A. Ultramicroscopy, Vol. 98, Issue 2-4 https://doi.org/10.1016/j.ultramic.2003.08.023	journal	January 2004
Contributions to the contrast in experimental high-angle annular dark-field images Klenov, Dmitri O.; Stemmer, Susanne Ultramicroscopy, Vol. 106, Issue 10, p. 889-901 https://doi.org/10.1016/j.ultramic.2006.03.007	journal	August 2006
An efficient way of including thermal diffuse scattering in simulation of scanning transmission electron microscopic images Croitoru, M. D.; Van Dyck, D.; Van Aert, S. Ultramicroscopy, Vol. 106, Issue 10 https://doi.org/10.1016/j.ultramic.2006.04.006	journal	August 2006
An emission-potential multislice approximation to simulate thermal diffuse scattering in high-resolution transmission electron microscopy Rosenauer, Andreas; Schowalter, Marco; Titantah, John T. Ultramicroscopy, Vol. 108, Issue 12 https://doi.org/10.1016/j.ultramic.2008.04.002	journal	November 2008
Experimental quantification of annular dark-field images in scanning transmission electron microscopy LeBeau, James M.; Stemmer, Susanne Ultramicroscopy, Vol. 108, Issue 12 https://doi.org/10.1016/j.ultramic.2008.07.001	journal	November 2008
Quantitative atomic resolution mapping using high-angle annular dark field scanning transmission electron microscopy Van Aert, S.; Verbeeck, J.; Erni, R. Ultramicroscopy, Vol. 109, Issue 10 https://doi.org/10.1016/j.ultramic.2009.05.010	journal	September 2009
Quantification of Sample Thickness and In-Concentration of InGaAs Quantum Wells by Transmission Measurements in a Scanning Electron Microscope Volkenandt, T.; Müller, E.; Hu, D. Z. Microscopy and Microanalysis, Vol. 16, Issue 5 https://doi.org/10.1017/S1431927610000292	journal	July 2010
Surface Channeling in Aberration-corrected STEM of Nanostructures Liu, J.; Allard, Lf Microscopy and Microanalysis, Vol. 16, Issue S2 https://doi.org/10.1017/S143192761005991X	journal	July 2010
Atomic Resolution Imaging of Nanoscale Structural Ordering in a Complex Metal Oxide Catalyst Zhu, Yihan; Wang, Qingxiao; Zhao, Lan Chemistry of Materials, Vol. 24, Issue 16 https://doi.org/10.1021/cm301828n	journal	August 2012
Using Aberration-Corrected STEM Imaging to Explore Chemical and Structural Variations in the M1 Phase of the MoVNbTeO Oxidation Catalyst Pyrz, William D.; Blom, Douglas A.; Shiju, N. Raveendran The Journal of Physical Chemistry C, Vol. 112, Issue 27 https://doi.org/10.1021/jp801584m	journal	June 2008
Multifunctionality of Active Centers in (Amm)oxidation Catalysts: From Bi–Mo–O_x to Mo–V–Nb–(Te, Sb)–O_x Grasselli, Robert K.; Burrington, James D.; Buttrey, Douglas J. Topics in Catalysis, Vol. 23, Issue 1/4, p. 5-22 https://doi.org/10.1023/A:1024859917786	journal	August 2003
Chemically sensitive structure-imaging with a scanning transmission electron microscope Pennycook, S. J.; Boatner, L. A. Nature, Vol. 336, Issue 6199 https://doi.org/10.1038/336565a0	journal	December 1988
Chapter 4. Propane-Selective Oxidation to Acrylic Acid Trunschke, Annette Nanostructured Catalysts https://doi.org/10.1039/9781847559876-00056	book	January 2011
Quantitative Z-contrast atomic resolution studies of semiconductor nanostructured materials Carlino, E. Journal of Physics: Conference Series, Vol. 209 https://doi.org/10.1088/1742-6596/209/1/012005	journal	February 2010
Quantitative STEM: Experimental Methods and Applications LeBeau, J. M.; Findlay, S. D.; Allen, L. J. Journal of Physics: Conference Series, Vol. 371 https://doi.org/10.1088/1742-6596/371/1/012053	journal	July 2012
High-angle scattering of fast electrons from crystals containing heavy elements: Simulation and experiment LeBeau, James M.; Findlay, Scott D.; Wang, Xiqu Physical Review B, Vol. 79, Issue 21 https://doi.org/10.1103/PhysRevB.79.214110	journal	June 2009
Quantitative Atomic Resolution Scanning Transmission Electron Microscopy LeBeau, James M.; Findlay, Scott D.; Allen, Leslie J. Physical Review Letters, Vol. 100, Issue 20 https://doi.org/10.1103/PhysRevLett.100.206101	journal	May 2008
High-resolution incoherent imaging of crystals Pennycook, S.; Jesson, D. Physical Review Letters, Vol. 64, Issue 8 https://doi.org/10.1103/PhysRevLett.64.938	journal	February 1990
Determination of Atomic Positions in a Solid Xe Precipitate Embedded in an Al Matrix Mitsuishi, K.; Kawasaki, M.; Takeguchi, M. Physical Review Letters, Vol. 82, Issue 15 https://doi.org/10.1103/PhysRevLett.82.3082	journal	April 1999
The `Frozen-Lattice' Approach for Incoherent Phonon Excitation in Electron Scattering. How Accurate Is It? Wang, Z. L. Acta Crystallographica Section A Foundations of Crystallography, Vol. 54, Issue 4 https://doi.org/10.1107/S0108767398001457	journal	July 1998
Image Contrast And Localized Signal Selection Techniques Howie, A. Journal of Microscopy, Vol. 117, Issue 1 https://doi.org/10.1111/j.1365-2818.1979.tb00228.x	journal	September 1979
Light Alkanes Oxidation: Targets Reached and Current Challenges Ivars, Francisco; Lopez Nieto, José M. Handbook of Advanced Methods and Processes in Oxidation Catalysis https://doi.org/10.1142/9781848167513_0024	book	August 2014

Similar Records

STEM HAADF Image Simulation of the Orthorhombic M1 Phase in the Mo-V-Nb-Te-O Propane Oxidation Catalyst

Journal Article · Fri Dec 30 23:00:00 EST 2011 · ChemCatChem · OSTI ID:1042275

Surface Termination of M1 Phase and Rational Design of Propane Ammoxidation Catalysts

Technical Report · Sun Feb 15 23:00:00 EST 2015 · OSTI ID:1170226

Propane ammoxidation over the Mo-V-Te-Nb-O M1 phase: Reactivity of surface cations in hydrogen abstraction steps

Journal Article · Fri Dec 31 23:00:00 EST 2010 · Topics in Catalysis · OSTI ID:1018265

Quantitative Analysis of HAADF–STEM Images of MoVTeTaO M1 Phase Catalyst for Propane Ammoxidation to Acrylonitrile

Citation Formats

References (48)

Similar Records

Related Subjects