Design and synthesis of highly active MoVTeNb-oxides for ethane oxidative dehydrogenation

Melzer, Daniel; Mestl, Gerhard; Wanninger, Klaus; Zhu, Yuanyuan; Browning, Nigel D.; Sanchez-Sanchez, Maricruz; Lercher, Johannes A.

doi:10.1038/s41467-019-11940-0

Design and synthesis of highly active MoVTeNb-oxides for ethane oxidative dehydrogenation

Journal Article · Thu Sep 05 00:00:00 EDT 2019 · Nature Communications

DOI:https://doi.org/10.1038/s41467-019-11940-0· OSTI ID:1624188

^[1]; Mestl, Gerhard ^[2]; Wanninger, Klaus ^[2]; Zhu, Yuanyuan ^[3]; Browning, Nigel D. ^[4]; Sanchez-Sanchez, Maricruz ^[5]; Lercher, Johannes A. ^[6]

Technical Univ. of Munich (Germany). Dept. of Chemie & Catalysis Research Center; DOE/OSTI
Clariant Produkte GmbH, Bruckmühl (Germany)
Univ. of Connecticut, Storrs, CT (United States). Inst. of Materials Science. Dept. of Materials Science and Engineering
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis; Univ. of Liverpool (United Kingdom). School of Engineering & School of Physical Sciences. Imaging Center at Liverpool (ICal)
Technical Univ. of Munich (Germany). Dept. of Chemie & Catalysis Research Center
Technical Univ. of Munich (Germany). Dept. of Chemie & Catalysis Research Center; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis

Ethane oxidative dehydrogenation (ODH) is an alternative route for ethene production. Crystalline M1 phase of Mo-V mixed metal oxide is an excellent catalyst for this reaction. Here we show a hydrothermal synthesis method that generates M1 phases with high surface areas starting from poorly soluble metal oxides. Use of organic additives allows control of the concentration of metals in aqueous suspension. Reactions leading to crystalline M1 take place at 190 °C, i.e., approximately 400 °C lower than under current synthesis conditions. The evolution of solvated polyoxometalate ions and crystalline phases in the solid is monitored by spectroscopies. Catalysts prepared by this route show higher ODH activity compared to conventionally prepared catalysts. The higher activity is due not only to the high specific surface area but also to the corrugated lateral termination of the M1 crystals, as seen by atomic resolution electron microscopy, exposing a high concentration of catalytically active sites.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER). Biological Systems Science Division

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1624188

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 10; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (43)

Aiding the Self-Assembly of Supramolecular Polyoxometalates under Hydrothermal Conditions To Give Precursors of Complex Functional Oxides Sanchez Sanchez, Maricruz; Girgsdies, Frank; Jastak, Mateusz Angewandte Chemie, Vol. 124, Issue 29 https://doi.org/10.1002/ange.201200746	journal	June 2012
Atomic-Scale Determination of Active Facets on the MoVTeNb Oxide M1 Phase and Their Intrinsic Catalytic Activity for Ethane Oxidative Dehydrogenation Melzer, Daniel; Xu, Pinghong; Hartmann, Daniela Angewandte Chemie, Vol. 128, Issue 31 https://doi.org/10.1002/ange.201600463	journal	March 2016
Synthesis of Orthorhombic Mo-V-Sb Oxide Species by Assembly of Pentagonal Mo ₆ O ₂₁ Polyoxometalate Building Blocks Sadakane, Masahiro; Yamagata, Keiko; Kodato, Katsunori Angewandte Chemie International Edition, Vol. 48, Issue 21 https://doi.org/10.1002/anie.200805792	journal	May 2009
Removing Compositional Boundaries in Mixed-Linker Keplerate Clusters Botar, Bogdan; Ellern, Arkady; Sougrati, Moulay T. European Journal of Inorganic Chemistry, Vol. 2009, Issue 34 https://doi.org/10.1002/ejic.200900638	journal	December 2009
Assembly of a Pentagonal Polyoxomolybdate Building Block, [Mo ₆ O ₂₁ ] ^6- , into Crystalline MoV Oxides Sadakane, Masahiro; Endo, Keisuke; Kodato, Katsunori European Journal of Inorganic Chemistry, Vol. 2013, Issue 10-11 https://doi.org/10.1002/ejic.201201142	journal	December 2012
Active centers, catalytic behavior, symbiosis and redox properties of MoV(Nb,Ta)TeO ammoxidation catalysts Grasselli, Robert K.; Buttrey, Douglas J.; Burrington, James D. Topics in Catalysis, Vol. 38, Issue 1-3 https://doi.org/10.1007/s11244-006-0066-x	journal	July 2006
Preparation of Phase-Pure M1 MoVTeNb Oxide Catalysts by Hydrothermal Synthesis—Influence of Reaction Parameters on Structure and Morphology Celaya Sanfiz, A.; Hansen, T. W.; Girgsdies, F. Topics in Catalysis, Vol. 50, Issue 1-4 https://doi.org/10.1007/s11244-008-9106-z	journal	June 2008
On the Role of the Vanadium Distribution in MoVTeNbO x Mixed Oxides for the Selective Catalytic Oxidation of Propane Naraschewski, F. N.; Jentys, A.; Lercher, J. A. Topics in Catalysis, Vol. 54, Issue 10-12 https://doi.org/10.1007/s11244-011-9686-x	journal	May 2011
Observation of Sublattice Disordering of the Catalytic Sites in a Complex Mo–V–Nb–Te–O Oxidation Catalyst Using High Temperature STEM Imaging Blom, Douglas A.; Vogt, Thomas; Allard, Larry F. Topics in Catalysis, Vol. 57, Issue 14-16 https://doi.org/10.1007/s11244-014-0278-4	journal	July 2014
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
Techno-Economic Analysis of Oxidative Dehydrogenation Options Maffia, Gennaro J.; Gaffney, Anne M.; Mason, Olivia M. Topics in Catalysis, Vol. 59, Issue 17-18 https://doi.org/10.1007/s11244-016-0677-9	journal	August 2016
Bulk mixed Mo–V–Te–O catalysts for propane oxidation to acrylic acid Guliants, Vadim V.; Bhandari, Rishabh; Al-Saeedi, Jamal N. Applied Catalysis A: General, Vol. 274, Issue 1-2 https://doi.org/10.1016/j.apcata.2004.05.049	journal	October 2004
On the nature of active sites in MoVTeO and MoVTeNbO catalysts: The influence of catalyst activation temperature Concepción, P.; Hernández, S.; Nieto, J. M. López Applied Catalysis A: General, Vol. 391, Issue 1-2 https://doi.org/10.1016/j.apcata.2010.05.011	journal	January 2011
Heptagonal channel micropore of orthorhombic Mo3VOx as catalysis field for the selective oxidation of ethane Ishikawa, Satoshi; Yi, Xiaodong; Murayama, Toru Applied Catalysis A: General, Vol. 474 https://doi.org/10.1016/j.apcata.2013.07.050	journal	March 2014
The structure and catalytic properties of amorphous phase in MoVTeO catalysts for propane ammoxidation Ishchenko, E. V.; Andrushkevich, T. V.; Popova, G. Ya. Applied Catalysis A: General, Vol. 476 https://doi.org/10.1016/j.apcata.2014.02.022	journal	April 2014
Performance of phase-pure M1 MoVNbTeO x catalysts by hydrothermal synthesis with different post-treatments for the oxidative dehydrogenation of ethane Chu, Bozhao; Truter, Lara; Nijhuis, T. A. Applied Catalysis A: General, Vol. 498 https://doi.org/10.1016/j.apcata.2015.03.039	journal	June 2015
In-situ X-ray diffraction study of phase crystallization from an amorphous MoVTeNb oxide catalyst precursor Girgsdies, Frank; Schlögl, Robert; Trunschke, Annette Catalysis Communications, Vol. 18 https://doi.org/10.1016/j.catcom.2011.11.009	journal	February 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 influence of Te-precursor in Mo-V-Te-O and Mo-V-Te-Nb-O catalysts on their catalytic behaviour in the selective propane oxidation Botella, P.; Concepción, P.; Nieto, J. M. López Catalysis Today, Vol. 99, Issue 1-2 https://doi.org/10.1016/j.cattod.2004.09.023	journal	January 2005
Catalysis field in orthorhombic Mo3VOx oxide catalyst for the selective oxidation of ethane, propane and acrolein Ishikawa, Satoshi; Yi, Xiaodong; Murayama, Toru Catalysis Today, Vol. 238 https://doi.org/10.1016/j.cattod.2013.12.054	journal	December 2014
Selective oxidative dehydrogenation of ethane on MoVTeNbO mixed metal oxide catalysts Botella, P. Journal of Catalysis, Vol. 225, Issue 2 https://doi.org/10.1016/j.jcat.2004.04.024	journal	July 2004
Mo-V-Te-(Nb)-O mixed metal oxides prepared by hydrothermal synthesis for catalytic selective oxidations of propane and propene to acrylic acid Vitry, D. Applied Catalysis A: General, Vol. 251, Issue 2 https://doi.org/10.1016/s0926-860x(03)00381-8	journal	September 2003
Structural Complexity in Heterogeneous Catalysis: Cataloging Local Nanostructures Masliuk, Liudmyla; Heggen, Marc; Noack, Johannes The Journal of Physical Chemistry C, Vol. 121, Issue 43 https://doi.org/10.1021/acs.jpcc.7b08333	journal	October 2017
Unit Synthesis Approach for Creating High Dimensionally Structured Complex Metal Oxides as Catalysts for Selective Oxidations Ishikawa, Satoshi; Zhang, Zhenxin; Ueda, Wataru ACS Catalysis, Vol. 8, Issue 4 https://doi.org/10.1021/acscatal.7b02244	journal	February 2018
Influence of Tight Confinement on Selective Oxidative Dehydrogenation of Ethane on MoVTeNb Mixed Oxides Annamalai, Leelavathi; Liu, Yilang; Ezenwa, Sopuruchukwu ACS Catalysis, Vol. 8, Issue 8 https://doi.org/10.1021/acscatal.8b01586	journal	July 2018
Better Catalysts through Microscopy: Mesoscale M1/M2 Intergrowth in Molybdenum–Vanadium Based Complex Oxide Catalysts for Propane Ammoxidation He, Qian; Woo, Jungwon; Belianinov, Alexei ACS Nano, Vol. 9, Issue 4 https://doi.org/10.1021/acsnano.5b00271	journal	February 2015
Atomic-level imaging of Mo-V-O complex oxide phase intergrowth, grain boundaries, and defects using HAADF-STEM Pyrz, W. D.; Blom, D. A.; Sadakane, M. Proceedings of the National Academy of Sciences, Vol. 107, Issue 14 https://doi.org/10.1073/pnas.1001239107	journal	March 2010
Archimedean Synthesis and Magic Numbers: “Sizing” Giant Molybdenum-Oxide-Based Molecular Spheres of the Keplerate Type Müller, Achim; Sarkar, Sabyasachi; Shah, Syed Qaiser Nazir Angewandte Chemie International Edition, Vol. 38, Issue 21 https://doi.org/10.1002/(SICI)1521-3773(19991102)38:21<3238::AID-ANIE3238>3.0.CO;2-6	journal	November 1999
Archimedean Synthesis and Magic Numbers: “Sizing” Giant Molybdenum-Oxide-Based Molecular Spheres of the Keplerate Type Müller, Achim; Sarkar, Sabyasachi; Shah, Syed Qaiser Nazir Angewandte Chemie International Edition, Vol. 38, Issue 21 https://doi.org/10.1002/(sici)1521-3773(19991102)38:21<3238::aid-anie3238>3.3.co;2-y	journal	November 1999
Synthesis of Orthorhombic Mo-V-Sb Oxide Species by Assembly of Pentagonal Mo ₆ O ₂₁ Polyoxometalate Building Blocks Sadakane, Masahiro; Yamagata, Keiko; Kodato, Katsunori Angewandte Chemie, Vol. 121, Issue 21 https://doi.org/10.1002/ange.200805792	journal	May 2009
Aiding the Self-Assembly of Supramolecular Polyoxometalates under Hydrothermal Conditions To Give Precursors of Complex Functional Oxides Sanchez Sanchez, Maricruz; Girgsdies, Frank; Jastak, Mateusz Angewandte Chemie International Edition, Vol. 51, Issue 29 https://doi.org/10.1002/anie.201200746	journal	June 2012
Atomic-Scale Determination of Active Facets on the MoVTeNb Oxide M1 Phase and Their Intrinsic Catalytic Activity for Ethane Oxidative Dehydrogenation Melzer, Daniel; Xu, Pinghong; Hartmann, Daniela Angewandte Chemie International Edition, Vol. 55, Issue 31 https://doi.org/10.1002/anie.201600463	journal	March 2016
MoVTeNbO Multifunctional Catalysts: Correlation Between Constituent Crystalline Phases and Catalytic Performance. Botella, P.; Garcia-Gonzalez, E.; Lopez Nieto, J. M. ChemInform, Vol. 36, Issue 34 https://doi.org/10.1002/chin.200534019	journal	August 2005
[{(Mo)Mo5O21(H2O)3 (SO4)}12(VO)30 (H2O)20]36-: A Molecular Quantum Spin Icosidodecahedron. Botar, Bogdan; Koegerler, Paul; Hill, Craig L. ChemInform, Vol. 36, Issue 41 https://doi.org/10.1002/chin.200541018	journal	October 2005
Active Sites for Propane Oxidation: Some Generic Considerations Schlögl, Robert Topics in Catalysis, Vol. 54, Issue 10-12 https://doi.org/10.1007/s11244-011-9683-0	journal	May 2011
Multi-dimensional Crystal Structuring of Complex Metal Oxide Catalysts of Group V and VI Elements by Unit-Assembling Ishikawa, Satoshi; Zhang, Zhenxin; Murayama, Toru Topics in Catalysis, Vol. 62, Issue 17-20 https://doi.org/10.1007/s11244-018-1077-0	journal	November 2018
Selective oxidation of light alkanes over hydrothermally synthesized Mo-V-M-O (M=Al, Ga, Bi, Sb, and Te) oxide catalysts Ueda, Wataru; Oshihara, Kenzo Applied Catalysis A: General, Vol. 200, Issue 1-2 https://doi.org/10.1016/S0926-860X(00)00627-X	journal	August 2000
Mo-V-Te-(Nb)-O mixed metal oxides prepared by hydrothermal synthesis for catalytic selective oxidations of propane and propene to acrylic acid Vitry, D. Applied Catalysis A: General, Vol. 251, Issue 2 https://doi.org/10.1016/S0926-860X(03)00381-8	journal	September 2003
MoVTeNbO multifunctional catalysts: Correlation between constituent crystalline phases and catalytic performance Botella, P.; García-González, E.; López Nieto, J. M. Solid State Sciences, Vol. 7, Issue 5 https://doi.org/10.1016/j.solidstatesciences.2005.01.012	journal	May 2005
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
The selective oxidative dehydrogenation of ethane over hydrothermally synthesised MoVTeNb catalysts Nieto, J. M. López; Botella, P.; Vázquez, M. I. Chem. Commun., Issue 17 https://doi.org/10.1039/B204037A	journal	January 2002
Reduction of vanadium(v) by oxalic acid in aqueous acid solutions Bruyère, Vivianne I. E.; García Rodenas, Luis A.; Morando, Pedro J. Journal of the Chemical Society, Dalton Transactions, Issue 24 https://doi.org/10.1039/b103320b	journal	November 2001
[{(Mo)Mo5O21(H2O)3(SO4)}12(VO)30(H2O)20]36–: A molecular quantum spin icosidodecahedron Botar, Bogdan; Kögerler, Paul; Hill, Craig L. Chemical Communications, Issue 25 https://doi.org/10.1039/b504491j	journal	January 2005

Similar Records

Process economics and safety considerations for the oxidative dehydrogenation of ethane using the M1 catalyst

Journal Article · Thu Nov 30 23:00:00 EST 2017 · Catalysis Today · OSTI ID:1361427

Intrinsic kinetic model for oxidative dehydrogenation of ethane over MoVTeNb mixed metal oxides: A mechanistic approach

Journal Article · Sat Feb 29 23:00:00 EST 2020 · Chemical Engineering Journal · OSTI ID:1647219

Oxidative Dehydrogenation of Ethane: A Chemical Looping Approach

Journal Article · Mon Jun 13 20:00:00 EDT 2016 · Energy Technology · OSTI ID:1533166

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Science & Technology - Other Topics

Design and synthesis of highly active MoVTeNb-oxides for ethane oxidative dehydrogenation

Citation Formats

References (43)

Similar Records

Related Subjects