Evaluating the accuracy of common γ-Al2O3 structure models by selected area electron diffraction from high-quality crystalline γ-Al2O3

Ayoola, Henry O.; House, Stephen D.; Bonifacio, Cecile S.; Kisslinger, Kim; Saidi, Wissam A.; Yang, Judith C.

doi:10.1016/j.actamat.2019.10.027

Evaluating the accuracy of common γ-Al₂O₃ structure models by selected area electron diffraction from high-quality crystalline γ-Al₂O₃

Journal Article · Wed Oct 30 00:00:00 EDT 2019 · Acta Materialia

DOI:https://doi.org/10.1016/j.actamat.2019.10.027· OSTI ID:1581957

^[1]; ^[1]; Bonifacio, Cecile S. ^[2]; Kisslinger, Kim ^[3]; Saidi, Wissam A. ^[1]; Yang, Judith C. ^[1]

Univ. of Pittsburgh, PA (United States)
Univ. of Pittsburgh, PA (United States); E.A. Fischione Instruments Inc., Export, PA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

Single crystal and textured polycrystalline γ-Al₂O₃ thin films were synthesized by oxidation of NiAl(110) in air at 850 °C for 1 and 2 hours, respectively, and used to evaluate the accuracy of two spinel-based and two nonspinel models by comparison of selected-area electron diffraction (SAED). The lattice interplanar distances derived from the polycrystalline SAED pattern most closely matched the cubic spinel γ-Al₂O₃ model. The single-crystal SAED spot pattern reflected symmetry consistent with both the cubic spinel and tetragonal nonspinel models, yet, the Al cation distribution better matched the cubic spinel model based on the relative intensities of diffraction spots. Our work indicates that the traditional cubic spinel model is a more accurate model of γ-Al₂O₃ than the other models considered. Furthermore, the spinel-based monoclinic model is more accurate than the monoclinic nonspinel model. The understanding of the relative accuracy of the different models is key for simulating γ-Al₂O₃ containing systems and is of general interest for the metal oxide and ceramic communities.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC0012704

OSTI ID:: 1581957

Report Number(s):: BNL--213512-2020-JAAM

Journal Information:: Acta Materialia, Journal Name: Acta Materialia Journal Issue: C Vol. 182; ISSN 1359-6454

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (56)

γ-Alumina as a Support for Catalysts: A Review of Fundamental Aspects Trueba, Monica; Trasatti, Stefano P. European Journal of Inorganic Chemistry, Vol. 2005, Issue 17 https://doi.org/10.1002/ejic.200500348	journal	September 2005
DiffTools: Electron diffraction software tools for DigitalMicrograph™ Mitchell, D. R. G. Microscopy Research and Technique, Vol. 71, Issue 8 https://doi.org/10.1002/jemt.20591	journal	August 2008
Transient oxidation of Single-Crystal β-NiAl Doychak, J.; Smialek, J. L.; Mitchell, T. E. Metallurgical Transactions A, Vol. 20, Issue 3 https://doi.org/10.1007/BF02653930	journal	March 1989
Atomistic study of vibrational properties of γ-Al2O3 Loyola, Claudia; Menéndez-Proupin, Eduardo; Gutiérrez, Gonzalo Journal of Materials Science, Vol. 45, Issue 18 https://doi.org/10.1007/s10853-010-4477-5	journal	April 2010
The dehydration of boehmite, γ-AlOOH, to γ-Al2O3 Wilson, S. J. Journal of Solid State Chemistry, Vol. 30, Issue 2 https://doi.org/10.1016/0022-4596(79)90106-3	journal	November 1979
Formation of a well-ordered aluminium oxide overlayer by oxidation of NiAl(110) Jaeger, R. M.; Kuhlenbeck, H.; Freund, H. -J. Surface Science, Vol. 259, Issue 3 https://doi.org/10.1016/0039-6028(91)90555-7	journal	December 1991
Electronic and crystallographic structure of γ-alumina thin films Ealet, B.; Elyakhloufi, M. H.; Gillet, E. Thin Solid Films, Vol. 250, Issue 1-2 https://doi.org/10.1016/0040-6090(94)90171-6	journal	October 1994
Transition alumina structures studied using HREM Morrissey, K. J.; Czanderna, K. K.; Merrill, R. P. Ultramicroscopy, Vol. 18, Issue 1-4 https://doi.org/10.1016/0304-3991(85)90156-1	journal	January 1985
Electron microscopy studies of NiAl/γ-Al2O3 interfaces Yang, J. C.; Nadarzinski, K.; Schumann, E. Scripta Metallurgica et Materialia, Vol. 33, Issue 7 https://doi.org/10.1016/0956-716X(95)00341-R	journal	October 1995
Distribution of tetrahedral and octahedral A1 sites in gamma alumina Lee, M. -H.; Cheng, Chi-Feng; Heine, Volker Chemical Physics Letters, Vol. 265, Issue 6 https://doi.org/10.1016/S0009-2614(96)01492-3	journal	February 1997
Electrolytic conduction of a solid insulator at high fields The formation of the anodic oxide film on aluminium Verwey, E. J. W. Physica, Vol. 2, Issue 1-12 https://doi.org/10.1016/S0031-8914(35)90193-8	journal	January 1935
Oxidation of NiAl and FeAl Grabke, H. J. Intermetallics, Vol. 7, Issue 10 https://doi.org/10.1016/S0966-9795(99)00037-0	journal	October 1999
Cubic to monoclinic phase transformations in alumina Levin, I.; Bendersky, L. A.; Brandon, D. G. Acta Materialia, Vol. 45, Issue 9 https://doi.org/10.1016/S1359-6454(97)00040-2	journal	September 1997
Transient oxidation of NiAl Yang, J. C.; Schumann, E.; Levin, I. Acta Materialia, Vol. 46, Issue 6 https://doi.org/10.1016/S1359-6454(97)00378-9	journal	March 1998
γ-Al2O3 thin film formation via oxidation of β-NiAl(110) Zhang, Zhongfan; Li, Long; Yang, Judith C. Acta Materialia, Vol. 59, Issue 15 https://doi.org/10.1016/j.actamat.2011.05.064	journal	September 2011
Deposition of alumina thin film by dual magnetron sputtering: Is it γ-Al2O3? Engelhart, W.; Dreher, W.; Eibl, O. Acta Materialia, Vol. 59, Issue 20 https://doi.org/10.1016/j.actamat.2011.08.048	journal	December 2011
On the role of oxocarbenium ions formed in Brønsted acidic condition on γ-Al2O3 surface in the ring-opening of γ-valerolactone Khan, Tuhin Suvra; Gupta, Shelaka; Bandodkar, Prasad Applied Catalysis A: General, Vol. 560 https://doi.org/10.1016/j.apcata.2018.04.035	journal	June 2018
Insight into the origin of sulfur tolerance of Ag/Al2O3 in the H2-C3H6-SCR of NOx Xu, Guangyan; Ma, Jinzhu; Wang, Lian Applied Catalysis B: Environmental, Vol. 244 https://doi.org/10.1016/j.apcatb.2018.11.050	journal	May 2019
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
Use of DFT to achieve a rational understanding of acid?basic properties of ?-alumina surfaces Digne, M. Journal of Catalysis, Vol. 226, Issue 1 https://doi.org/10.1016/j.jcat.2004.04.020	journal	August 2004
Regeneration of sulfur-poisoned Pd-based catalyst for natural gas oxidation Honkanen, Mari; Wang, Jianguang; Kärkkäinen, Marja Journal of Catalysis, Vol. 358 https://doi.org/10.1016/j.jcat.2017.12.021	journal	February 2018
Direct comparison between two structural models by DFT calculations Ferreira, Ary R.; Martins, Mateus J. F.; Konstantinova, Elena Journal of Solid State Chemistry, Vol. 184, Issue 5 https://doi.org/10.1016/j.jssc.2011.03.016	journal	May 2011
Structural analysis of highly porous γ-Al2O3 Samain, Louise; Jaworski, Aleksander; Edén, Mattias Journal of Solid State Chemistry, Vol. 217 https://doi.org/10.1016/j.jssc.2014.05.004	journal	September 2014
Study of Raman spectra for γ-Al2O3 models by using first-principles method Liu, Yong; Cheng, Bo; Wang, Kang-Kai Solid State Communications, Vol. 178 https://doi.org/10.1016/j.ssc.2013.09.030	journal	January 2014
Electron Diffraction Based Analysis of Phase Fractions and Texture in Nanocrystalline Thin Films, Part I: Principles Lábár, János L. Microscopy and Microanalysis, Vol. 14, Issue 4 https://doi.org/10.1017/S1431927608080380	journal	July 2008
Electron Diffraction Based Analysis of Phase Fractions and Texture in Nanocrystalline Thin Films, Part III: Application Examples Lábár, J. L.; Adamik, M.; Barna, B. P. Microscopy and Microanalysis, Vol. 18, Issue 2 https://doi.org/10.1017/S1431927611012803	journal	March 2012
Seeking a Structure–Function Relationship for γ-Al ₂ O ₃ Surfaces Acikgoz, Muhammed; Harrell, Jaren; Pavanello, Michele The Journal of Physical Chemistry C, Vol. 122, Issue 44 https://doi.org/10.1021/acs.jpcc.8b06506	journal	October 2018
CO ₂ Activation on Ni/γ–Al ₂ O ₃ Catalysts by First-Principles Calculations: From Ideal Surfaces to Supported Nanoparticles Silaghi, Marius-Christian; Comas-Vives, Aleix; Copéret, Christophe ACS Catalysis, Vol. 6, Issue 7 https://doi.org/10.1021/acscatal.6b00822	journal	June 2016
Structure–Activity Relationships in Alkane Dehydrogenation on γ-Al ₂ O ₃ : Site-Dependent Reactions Dixit, Mudit; Kostetskyy, Pavlo; Mpourmpakis, Giannis ACS Catalysis, Vol. 8, Issue 12 https://doi.org/10.1021/acscatal.8b03484	journal	October 2018
Boehmite Derived γ-Alumina System. 1. Structural Evolution with Temperature, with the Identification and Structural Determination of a New Transition Phase, γ‘-Alumina Paglia, Gianluca; Buckley, Craig E.; Rohl, Andrew L. Chemistry of Materials, Vol. 16, Issue 2 https://doi.org/10.1021/cm034917j	journal	January 2004
Fine-Scale Nanostructure in γ-Al ₂ O ₃ Paglia, Gianluca; Božin, Emil S.; Billinge, Simon J. L. Chemistry of Materials, Vol. 18, Issue 14 https://doi.org/10.1021/cm060277j	journal	July 2006
DRFT-IR Studies of the Surface of γ-Alumina Liu, Xinsheng; Truitt, Ralph E. Journal of the American Chemical Society, Vol. 119, Issue 41 https://doi.org/10.1021/ja971214s	journal	October 1997
Theoretical Study of the Dehydration Process of Boehmite to γ-Alumina Krokidis, Xénophon; Raybaud, Pascal; Gobichon, Anne-Elisabeth The Journal of Physical Chemistry B, Vol. 105, Issue 22 https://doi.org/10.1021/jp0038310	journal	June 2001
Examination of Spinel and Nonspinel Structural Models for γ-Al ₂ O ₃ by DFT and Rietveld Refinement Simulations Sun, Mingyong; Nelson, Alan E.; Adjaye, John The Journal of Physical Chemistry B, Vol. 110, Issue 5 https://doi.org/10.1021/jp056465z	journal	February 2006
Comment on “Examination of Spinel and Nonspinel Structural Models for γ-Al ₂ O ₃ by DFT and Rietveld Refinement Simulations” Digne, Mathieu; Raybaud, Pascal; Sautet, Philippe The Journal of Physical Chemistry B, Vol. 110, Issue 41 https://doi.org/10.1021/jp061466s	journal	October 2006
Comment on “Examination of Spinel and Nonspinel Structural Models for γ-Al ₂ O ₃ by DFT and Rietveld Refinement Simulations” Paglia, Gianluca; Buckley, C. E.; Rohl, Andrew L. The Journal of Physical Chemistry B, Vol. 110, Issue 41 https://doi.org/10.1021/jp061648m	journal	October 2006
Tomography and High-Resolution Electron Microscopy Study of Surfaces and Porosity in a Plate-like γ-Al ₂ O ₃ Kovarik, Libor; Genc, Arda; Wang, Chongmin The Journal of Physical Chemistry C, Vol. 117, Issue 1 https://doi.org/10.1021/jp306800h	journal	December 2012
Role of Pentacoordinated Al ³⁺ Ions in the High Temperature Phase Transformation of γ-Al ₂ O ₃ Kwak, Ja Hun; Hu, Jianzhi; Lukaski, Adrienne The Journal of Physical Chemistry C, Vol. 112, Issue 25 https://doi.org/10.1021/jp802631u	journal	May 2008
A crystal structure determined with 0.02 Å accuracy by electron microscopy Weirich, Thomas E.; Ramlau, Reiner; Simon, Arndt Nature, Vol. 382, Issue 6587 https://doi.org/10.1038/382144a0	journal	July 1996
Quantum-chemical study of stable, meta-stable and high-pressure alumina polymorphs and aluminum hydroxides Peintinger, Michael F.; Kratz, Michael J.; Bredow, Thomas J. Mater. Chem. A, Vol. 2, Issue 32 https://doi.org/10.1039/C4TA02663B	journal	January 2014
Optimal and near‐optimal filters in high‐resolution electron microscopy Kilaas, R. Journal of Microscopy, Vol. 190, Issue 1‐2 https://doi.org/10.1046/j.1365-2818.1998.3070861.x	journal	April 1998
The nature of hydrogen in γ-alumina Li, Yunguo; Lousada, Cláudio M.; Korzhavyi, Pavel A. Journal of Applied Physics, Vol. 115, Issue 20 https://doi.org/10.1063/1.4879897	journal	May 2014
Phase stability and structure of spinel-based transition aluminas Wolverton, C.; Hass, K. C. Physical Review B, Vol. 63, Issue 2 https://doi.org/10.1103/PhysRevB.63.024102	journal	December 2000
Theoretical structure determination of γ − Al 2 O 3 Gutiérrez, Gonzalo; Taga, Adrian; Johansson, Börje Physical Review B, Vol. 65, Issue 1 https://doi.org/10.1103/PhysRevB.65.012101	journal	November 2001
Phase transformation mechanism between γ- and θ-alumina Cai, Shu-Hui; Rashkeev, Sergey N.; Pantelides, Sokrates T. Physical Review B, Vol. 67, Issue 22 https://doi.org/10.1103/PhysRevB.67.224104	journal	June 2003
Tetragonal structure model for boehmite-derived γ-alumina Paglia, G.; Buckley, C. E.; Rohl, A. L. Physical Review B, Vol. 68, Issue 14 https://doi.org/10.1103/PhysRevB.68.144110	journal	October 2003
Ab initio study of γ − Al 2 O 3 surfaces Pinto, Henry P.; Nieminen, R. M.; Elliott, Simon D. Physical Review B, Vol. 70, Issue 12 https://doi.org/10.1103/PhysRevB.70.125402	journal	September 2004
Determination of the structure of γ -alumina from interatomic potential and first-principles calculations: The requirement of significant numbers of nonspinel positions to achieve an accurate structural model Paglia, Gianluca; Rohl, Andrew L.; Buckley, Craig E. Physical Review B, Vol. 71, Issue 22 https://doi.org/10.1103/PhysRevB.71.224115	journal	June 2005
Ab initio study of the physical properties of γ -Al 2 O 3 : Lattice dynamics, bulk properties, electronic structure, bonding, optical properties, and ELNES/XANES spectra Ching, W. Y.; Ouyang, Lizhi; Rulis, Paul Physical Review B, Vol. 78, Issue 1 https://doi.org/10.1103/PhysRevB.78.014106	journal	July 2008
Atomic Structure of a Spinel-Like Transition Al 2 O 3 ( 100 ) Surface Jensen, Thomas N.; Meinander, Kristoffer; Helveg, Stig Physical Review Letters, Vol. 113, Issue 10 https://doi.org/10.1103/PhysRevLett.113.106103	journal	September 2014
γ-Alumina: a single-crystal X-ray diffraction study Smrčok, Ľubomír; Langer, Vratislav; Křesťan, Jan Acta Crystallographica Section C Crystal Structure Communications, Vol. 62, Issue 9 https://doi.org/10.1107/S0108270106026850	journal	August 2006
Structures and transformation mechanisms of the η, γ and θ transition aluminas Zhou, R. S.; Snyder, R. L. Acta Crystallographica Section B Structural Science, Vol. 47, Issue 5 https://doi.org/10.1107/S0108768191002719	journal	October 1991
Study of phase transformations during calcination of aluminum hydroxides by selected area electron diffraction Lippens, B. C.; de Boer, J. H. Acta Crystallographica, Vol. 17, Issue 10 https://doi.org/10.1107/S0365110X64003267	journal	October 1964
Metastable Alumina Polymorphs: Crystal Structures and Transition Sequences Levin, Igor; Brandon, David Journal of the American Ceramic Society, Vol. 81, Issue 8 https://doi.org/10.1111/j.1151-2916.1998.tb02581.x	journal	August 1998
Coordinatively Unsaturated Al3+ Centers as Binding Sites for Active Catalyst Phases of Platinum on -Al2O3 Kwak, J. H.; Hu, J.; Mei, D. Science, Vol. 325, Issue 5948 https://doi.org/10.1126/science.1176745	journal	September 2009
Standard transition aluminas. Electron microscopy studies Santos, P. Souza; Santos, H. Souza; Toledo, S. P. Materials Research, Vol. 3, Issue 4 https://doi.org/10.1590/S1516-14392000000400003	journal	October 2000

Similar Records

Determination of the vacancy distribution over Al cation sites in γ-Al₂O₃

Journal Article · Thu Dec 21 19:00:00 EST 2023 · Materials Advances · OSTI ID:2251551

Examination of Spinel and Nonspinel Structural Models for gamma-Al2O3 by DFT and Rietveld Refinement Simulations

Journal Article · Sat Dec 31 23:00:00 EST 2005 · J. Phys. Chem. B · OSTI ID:914006

Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY
Crystalline oxides
Diffraction
Electron diffraction pattern
Transmission electron microscopy (TEM)
γ-Al2O3

Evaluating the accuracy of common γ-Al2O3 structure models by selected area electron diffraction from high-quality crystalline γ-Al2O3

Citation Formats

References (56)

Similar Records

Related Subjects

Evaluating the accuracy of common γ-Al₂O₃ structure models by selected area electron diffraction from high-quality crystalline γ-Al₂O₃