Structure analysis of supported disordered molybdenum oxides using pair distribution function analysis and automated cluster modelling

Lindahl Christiansen, Troels; Kjær, Emil T. S.; Kovyakh, Anton; Röderen, Morten L.; Høj, Martin; Vosch, Tom; Jensen, Kirsten M. Ø.

doi:10.1107/S1600576719016832

Title: Structure analysis of supported disordered molybdenum oxides using pair distribution function analysis and automated cluster modelling

Journal Article · 01 February 2020 · Journal of Applied Crystallography (Online)

DOI: https://doi.org/10.1107/S1600576719016832 · OSTI ID:1617955

Lindahl Christiansen, Troels; Kjær, Emil T. S.; Kovyakh, Anton; Röderen, Morten L.; Høj, Martin; Vosch, Tom;

Molybdenum oxides and sulfides on various low-cost high-surface-area supports are excellent catalysts for several industrially relevant reactions. The surface layer structure of these materials is, however, difficult to characterize due to small and disordered MoO _x domains. Here, it is shown how X-ray total scattering can be applied to gain insights into the structure through differential pair distribution function (d-PDF) analysis, where the scattering signal from the support material is subtracted to obtain structural information on the supported structure. MoO _x catalysts supported on alumina nanoparticles and on zeolites are investigated, and it is shown that the structure of the hydrated molybdenum oxide layer is closely related to that of disordered and polydisperse polyoxometalates. By analysing the PDFs with a large number of automatically generated cluster structures, which are constructed in an iterative manner from known polyoxometalate clusters, information is derived on the structural motifs in supported MoO _x .

View Journal Article

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1617955

Journal Information:: Journal of Applied Crystallography (Online), Journal Name: Journal of Applied Crystallography (Online) Journal Issue: 1 Vol. 53; ISSN JACGAR; ISSN 1600-5767

Publisher:: International Union of Crystallography (IUCr)Copyright Statement

Country of Publication:: Denmark

Language:: English

References (54)

Polyoxometalate Chemistry: An Old Field with New Dimensions in Several Disciplines Pope, Michael T.; Müller, Achim Angewandte Chemie International Edition in English, Vol. 30, Issue 1 https://doi.org/10.1002/anie.199100341	journal	January 1991
Determination of molybdenum-oxygen bond distances and bond orders by Raman spectroscopy Hardcastle, Franklin D.; Wachs, Israel E. Journal of Raman Spectroscopy, Vol. 21, Issue 10 https://doi.org/10.1002/jrs.1250211009	journal	October 1990
Molecular structures of supported metal oxide catalysts under different environments: Molecular structures of supported metal oxide catalysts Bañares, M. A.; Wachs, I. E. Journal of Raman Spectroscopy, Vol. 33, Issue 5 https://doi.org/10.1002/jrs.866	journal	May 2002
Methane Dehydro-aromatization under Nonoxidative Conditions over Mo/HZSM-5 Catalysts: EPR Study of the Mo Species on/in the HZSM-5 Zeolite Ma, Ding; Shu, Yuying; Bao, Xinhe Journal of Catalysis, Vol. 189, Issue 2 https://doi.org/10.1006/jcat.1999.2704	journal	January 2000
Structure and Properties of Oxidative Dehydrogenation Catalysts Based on MoO3/Al2O3 Chen, Kaidong; Xie, Shuibo; Bell, Alexis T. Journal of Catalysis, Vol. 198, Issue 2 https://doi.org/10.1006/jcat.2000.3125	journal	March 2001
Activity of Molybdenum Oxide Catalyst Supported on Al2O3, TiO2, and SiO2 Matrix in the Oxidative Dehydrogenation of n-Butane Setnička, Michal; Tišler, Zdeněk; Kubička, David Topics in Catalysis, Vol. 58, Issue 14-17 https://doi.org/10.1007/s11244-015-0453-2	journal	August 2015
Multiwavelength Raman Spectroscopic Characterization of Alumina-Supported Molybdenum Oxide Prepared by Vapor Deposition Drake, Tasha L.; Stair, Peter C. Topics in Catalysis, Vol. 60, Issue 19-20 https://doi.org/10.1007/s11244-017-0842-9	journal	November 2017
Characterization of supported molybdate catalysts during preparation using laser Raman spectroscopy Cheng, C. Journal of Catalysis, Vol. 60, Issue 2 https://doi.org/10.1016/0021-9517(79)90149-0	journal	November 1979
Crystallographic study of the ammonium/potassium 12-molybdophosphate ion-exchange system Boeyens, J. C. A.; McDougal, Gloria J.; Van R. Smit, J. Journal of Solid State Chemistry, Vol. 18, Issue 2 https://doi.org/10.1016/0022-4596(76)90095-5	journal	June 1976
Raman and IR studies of surface metal oxide species on oxide supports: Supported metal oxide catalysts Wachs, Israel E. Catalysis Today, Vol. 27, Issue 3-4 https://doi.org/10.1016/0920-5861(95)00203-0	journal	February 1996
Supported metal oxide and other catalysts for ethane conversion: a review Bañares, Miguel A. Catalysis Today, Vol. 51, Issue 2 https://doi.org/10.1016/S0920-5861(99)00053-X	journal	June 1999
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
Structure of alumina supported vanadia catalysts for oxidative dehydrogenation of propane prepared by flame spray pyrolysis Høj, Martin; Jensen, Anker D.; Grunwaldt, Jan-Dierk Applied Catalysis A: General, Vol. 451 https://doi.org/10.1016/j.apcata.2012.09.037	journal	January 2013
Structure, activity and kinetics of supported molybdenum oxide and mixed molybdenum–vanadium oxide catalysts prepared by flame spray pyrolysis for propane OHD Høj, Martin; Kessler, Thomas; Beato, Pablo Applied Catalysis A: General, Vol. 472 https://doi.org/10.1016/j.apcata.2013.11.027	journal	February 2014
Oxidative dehydrogenation of ethane and propane: How far from commercial implementation? Cavani, F.; Ballarini, N.; Cericola, A. Catalysis Today, Vol. 127, Issue 1-4, p. 113-131 https://doi.org/10.1016/j.cattod.2007.05.009	journal	September 2007
Structure and acidity of Mo/ZSM-5 synthesized by solid state reaction for methane dehydrogenation and aromatization Li, Bin; Li, Shijie; Li, Neng Microporous and Mesoporous Materials, Vol. 88, Issue 1-3 https://doi.org/10.1016/j.micromeso.2005.09.016	journal	January 2006
Mechanisms for Tungsten Oxide Nanoparticle Formation in Solvothermal Synthesis: From Polyoxometalates to Crystalline Materials Juelsholt, Mikkel; Lindahl Christiansen, Troels; Jensen, Kirsten M. Ø. The Journal of Physical Chemistry C, Vol. 123, Issue 8 https://doi.org/10.1021/acs.jpcc.8b12395	journal	February 2019
Core–Shell Nanostructured Catalysts Zhang, Qiao; Lee, Ilkeun; Joo, Ji Bong Accounts of Chemical Research, Vol. 46, Issue 8 https://doi.org/10.1021/ar300230s	journal	December 2012
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
Recent Developments in the Synthesis of Supported Catalysts Munnik, Peter; de Jongh, Petra E.; de Jong, Krijn P. Chemical Reviews, Vol. 115, Issue 14 https://doi.org/10.1021/cr500486u	journal	June 2015
Differential Pair Distribution Function Study of the Structure of Arsenate Adsorbed on Nanocrystalline γ-Alumina Li, Wei; Harrington, Richard; Tang, Yuanzhi Environmental Science & Technology, Vol. 45, Issue 22 https://doi.org/10.1021/es200750b	journal	November 2011
Investigation of Surface Structures by Powder Diffraction: A Differential Pair Distribution Function Study on Arsenate Sorption on Ferrihydrite Harrington, Richard; Hausner, Douglas B.; Bhandari, Narayan Inorganic Chemistry, Vol. 49, Issue 1 https://doi.org/10.1021/ic9022695	journal	January 2010
Predicting molecular structures of surface metal oxide species on oxide supports under ambient conditions Deo, Goutam; Wachs, Israel E. The Journal of Physical Chemistry, Vol. 95, Issue 15 https://doi.org/10.1021/j100168a033	journal	July 1991
Spectroscopic characterization of molybdenum oxalate in solution and on alumina Ng, K. Y. S.; Zhou, X.; Gulari, E. The Journal of Physical Chemistry, Vol. 89, Issue 12 https://doi.org/10.1021/j100258a011	journal	June 1985
Crystal structure and structure-related properties of ZSM-5 Olson, D. H.; Kokotailo, G. T.; Lawton, S. L. The Journal of Physical Chemistry, Vol. 85, Issue 15 https://doi.org/10.1021/j150615a020	journal	July 1981
Elucidating the Structure of Surface Acid Sites on γ-Al ₂ O ₃ Chupas, Peter J.; Chapman, Karena W.; Halder, Gregory J. Journal of the American Chemical Society, Vol. 133, Issue 22 https://doi.org/10.1021/ja2029574	journal	June 2011
The Electronic Structure and Stability of the Isomers of Octamolybdate Bridgeman, Adam J. The Journal of Physical Chemistry A, Vol. 106, Issue 50 https://doi.org/10.1021/jp027037l	journal	December 2002
Molecular Structural Determination of Molybdena in Different Environments: Aqueous Solutions, Bulk Mixed Oxides, and Supported MoO ₃ Catalysts Tian, Hanjing; Roberts, Charles A.; Wachs, Israel E. The Journal of Physical Chemistry C, Vol. 114, Issue 33 https://doi.org/10.1021/jp103269w	journal	July 2010
Measuring Correlated Atomic Motion Using X-ray Diffraction Jeong, Il-Kyoung; Proffen, Thomas; Mohiuddin-Jacobs, Farida The Journal of Physical Chemistry A, Vol. 103, Issue 7 https://doi.org/10.1021/jp9836978	journal	February 1999
Ab initio determination of solid-state nanostructure Juhás, P.; Cherba, D. M.; Duxbury, P. M. Nature, Vol. 440, Issue 7084 https://doi.org/10.1038/nature04556	journal	March 2006
Polymorphism in magic-sized Au144(SR)60 clusters Jensen, Kirsten M. Ø.; Juhas, Pavol; Tofanelli, Marcus A. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11859	journal	June 2016
Nanostructured materials for applications in heterogeneous catalysis Zaera, Francisco Chem. Soc. Rev., Vol. 42, Issue 7 https://doi.org/10.1039/C2CS35261C	journal	January 2013
Crystal structure of the heptamolybdate( VI )(paramolybdate) ion, [Mo ₇ O ₂₄ ] ^6– , in the ammonium and potassium tetrahydrate salts Evans, Howard T.; Gatehouse, Bryan M.; Leverett, Peter J. Chem. Soc., Dalton Trans., Issue 6 https://doi.org/10.1039/DT9750000505	journal	January 1975
Structure of intrazeolite molybdenum oxide clusters and their catalysis of the oxidation of ethyl alcohol Okamoto, Yasuaki; Oshima, Nobuyuki; Kobayashi, Yasuhiro Physical Chemistry Chemical Physics, Vol. 4, Issue 12 https://doi.org/10.1039/b108639c	journal	May 2002
Beyond crystallography: the study of disorder, nanocrystallinity and crystallographically challenged materials with pair distribution functions Billinge, Simon J. L.; Kanatzidis, M. G. Chemical Communications, Issue 7 https://doi.org/10.1039/b309577k	journal	January 2004
Direct observation of adsorbed H2-framework interactions in the Prussian Blue analogue MnII3[CoIII(CN)6]2: The relative importance of accessible coordination sites and van der Waals interactions Chapman, Karena W.; Chupas, Peter J.; Maxey, Evan R. Chemical Communications, Issue 38 https://doi.org/10.1039/b607250j	journal	January 2006
Structure and function of oxide nanostructures: catalytic consequences of size and composition Macht, Josef; Iglesia, Enrique Physical Chemistry Chemical Physics, Vol. 10, Issue 35 https://doi.org/10.1039/b805251d	journal	January 2008
On the configuration, molecular structure and vibrational properties of MoOx sites on alumina, zirconia, titania and silica Tsilomelekis, George; Boghosian, Soghomon Catalysis Science & Technology, Vol. 3, Issue 8 https://doi.org/10.1039/c3cy00057e	journal	January 2013
Raman Spectroscopy of Monolayer-Type Catalysts: Supported Molybdenum Oxides Mestl, Gerhard; Srinivasan, T. K. K. Catalysis Reviews, Vol. 40, Issue 4 https://doi.org/10.1080/01614949808007114	journal	November 1998
DIOPTAS : a program for reduction of two-dimensional X-ray diffraction data and data exploration Prescher, Clemens; Prakapenka, Vitali B. High Pressure Research, Vol. 35, Issue 3 https://doi.org/10.1080/08957959.2015.1059835	journal	May 2015
PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals Farrow, C. L.; Juhas, P.; Liu, J. W. Journal of Physics: Condensed Matter, Vol. 19, Issue 33 https://doi.org/10.1088/0953-8984/19/33/335219	journal	July 2007
The Structure and Formula of 12-Phosphotungstic Acid Keggin, J. F. Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 144, Issue 851 https://doi.org/10.1098/rspa.1934.0035	journal	March 1934
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
Rapid-acquisition pair distribution function (RA-PDF) analysis Chupas, Peter J.; Qiu, Xiangyun; Hanson, Jonathan C. Journal of Applied Crystallography, Vol. 36, Issue 6, p. 1342-1347 https://doi.org/10.1107/S0021889803017564	journal	November 2003
Finite size effects on the real-space pair distribution function of nanoparticles Gilbert, Benjamin Journal of Applied Crystallography, Vol. 41, Issue 3 https://doi.org/10.1107/S0021889808007905	journal	May 2008
Die Kristallstruktur des polymeren Oktamolybdats, (NH ₄ ) ₆ Mo ₈ O ₂₇ .4H ₂ O Böschen, I.; Buss, B.; Krebs, B. Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 30, Issue 1 https://doi.org/10.1107/S0567740874002184	journal	January 1974
Structure d'un paratungstate d'ammonium (NH ₄ ) ₆ H ₆ W ₁₂ O ₄₂ .10H ₂ O Averbuch-Pouchot, M. T.; Tordjman, I.; Durif, A. Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 35, Issue 7 https://doi.org/10.1107/S0567740879007378	journal	July 1979
Bis[2,2′-(butane-1,4-diyl)bis(1 H -benzimidazolium)] α-octamolybdate(VI) Wang, Li-Jun; Jiang, Hong; Wang, Yong Acta Crystallographica Section E Structure Reports Online, Vol. 63, Issue 2 https://doi.org/10.1107/S1600536807003017	journal	January 2007
Modelling pair distribution functions (PDFs) of organic compounds: describing both intra- and intermolecular correlation functions in calculated PDFs Prill, Dragica; Juhás, Pavol; Schmidt, Martin U. Journal of Applied Crystallography, Vol. 48, Issue 1 https://doi.org/10.1107/S1600576714026454	journal	January 2015
Complex modeling: a strategy and software program for combining multiple information sources to solve ill posed structure and nanostructure inverse problems Juhás, Pavol; Farrow, Christopher L.; Yang, Xiaohao Acta Crystallographica Section A Foundations and Advances, Vol. 71, Issue 6, p. 562-568 https://doi.org/10.1107/S2053273315014473	journal	September 2015
100 years of Debye's scattering equation Gelisio, Luca; Scardi, Paolo Acta Crystallographica Section A Foundations and Advances, Vol. 72, Issue 6 https://doi.org/10.1107/S2053273316014881	journal	October 2016
The Impact of Nanoscience on Heterogeneous Catalysis Bell, A. T. Science, Vol. 299, Issue 5613 https://doi.org/10.1126/science.1083671	journal	March 2003
Identification of molybdenum oxide nanostructures on zeolites for natural gas conversion Gao, J.; Zheng, Y.; Jehng, J. -M. Science, Vol. 348, Issue 6235 https://doi.org/10.1126/science.aaa7048	journal	April 2015
Differential Controls Over Tactile Detection in Humans by Motor Commands and Peripheral Reafference Chapman, C. Elaine; Beauchamp, Evelyne Journal of Neurophysiology, Vol. 96, Issue 3 https://doi.org/10.1152/jn.00214.2006	journal	September 2006

Similar Records

Molecular structures and reactivity of supported molybdenum oxide catalysts

Journal Article · 1994 · Journal of Catalysis · OSTI ID:98922

Kim, D S; Wachs, I E; Segawa, Kohichi

THE OXIDATION OF MOLYBDENUM

Journal Article · 1958 · Corrosion · OSTI ID:4341254

Jones, E S; Mosher, J F; Speiser, R; +1 more

Skeletal isomerization of hydrocarbons on molybdenum catalysts. I. X-ray photoelectron spectroscopy study of alumina-supported catalysts

Journal Article · 1987 · J. Catal.; (United States) · OSTI ID:5451522

Holl, Y; Touroude, R; Maire, G; +3 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
automated modelling
molybdenum oxides
nanostructure
pair distribution function analysis
supported catalysts

Title: Structure analysis of supported disordered molybdenum oxides using pair distribution function analysis and automated cluster modelling

Citation Formats

References (54)

Similar Records

Related Subjects