Computational Modeling of the Nature and Role of Ga Species for Light Alkane Dehydrogenation Catalyzed by Ga/H-MFI

Mansoor, Erum; Head-Gordon, Martin; Bell, Alexis T.

doi:10.1021/acscatal.7b04295

Title: Computational Modeling of the Nature and Role of Ga Species for Light Alkane Dehydrogenation Catalyzed by Ga/H-MFI

Journal Article · Tue May 15 00:00:00 EDT 2018 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.7b04295· OSTI ID:1571106

Mansoor, Erum ^[1];

^[2];

^[1]

Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
Univ. of California, Berkeley, CA (United States). Dept. of Chemistry

Ga-exchanged H-MFI zeolites are highly active for the dehydrogenation of light alkanes; however, both the nature of the active gallium species and the associated dehydrogenation mechanism have been difficult to establish. In this study, we examine the activity of Ga species in Ga/H-MFI by calculating the free energy landscapes on which all reactions occur. To this end, we use a hybrid quantum mechanics/molecular mechanics model for all electronic structure calculations. Quantum chemical calculations were carried out with a range-corrected functional and a good representation of dispersive interactions. The molecular mechanics part of our approach captures the long-range effects of Coulombic and dispersive interactions due to atoms in the extended framework. The rate-determining TS (RDTS) is identified by analysis of the free energy landscape for each mechanism, using the energetic span model. Our analysis reveals that, for reduced Ga/H-MFI, univalent and divalent gallium hydrides, [GaH₂]⁺ and [GaH]²⁺, respectively, are more active for ethane dehydrogenation in comparison to H⁺ sites and Ga⁺ sites. [GaH]²⁺ sites consistently emerge as the most active sites for light alkane dehydrogenation, providing significant enthalpic stabilization to C-H cleavage TSs via alkyl and carbenium dehydrogenation routes. In contrast, carbenium-like C-H cleavage TSs occurring on Brønsted acid sites are enthalpically less favorable due to their limited electronic interactions with framework O atoms and H⁺ sites. Activation enthalpy barriers for dehydrogenation determined using the energetic span analysis are in good agreement with those measured experimentally. Accounting for entropy of activation reveals that constrained TSs become less favorable in free energy with increasing chain length. Here, we also find that an increase in enthalpic favorability of the alkyl mechanism is observed with increasing chain length for the TS responsible for the second C-H cleavage step leading to alkene formation.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1571106

Journal Information:: ACS Catalysis, Vol. 8, Issue 7; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 71 works

Citation information provided by
Web of Science

References (70)

Catalytic Conversion of LPG to High-Value Aromatics: The Current State of the Art and Future Predictions Al-Zahrani, S. M. Developments in Chemical Engineering and Mineral Processing, Vol. 6, Issue 1-2 https://doi.org/10.1002/apj.5500060107	journal	January 1998
Monomolecular Conversion of Light Alkanes over H-ZSM-5 Narbeshuber, T. F.; Vinek, H.; Lercher, J. A. Journal of Catalysis, Vol. 157, Issue 2 https://doi.org/10.1006/jcat.1995.1304	journal	December 1995
Propane Aromatization over HZSM‐5 and Ga/HZSM‐5 Catalysts Bhan, Aditya; Nicholas Delgass, W. Catalysis Reviews, Vol. 50, Issue 1 https://doi.org/10.1080/01614940701804745	journal	February 2008
Transformation of Lower Alkanes into Aromatic Hydrocarbons over ZSM-5 Zeolites Ono, Yoshio Catalysis Reviews, Vol. 34, Issue 3 https://doi.org/10.1080/01614949208020306	journal	August 1992
Kinetic modeling of propane aromatization reaction over HZSM-5 and GaHZSM-5 Lukyanov, Dmitri B.; Gnep, N. Suor; Guisnet, Michel R. Industrial & Engineering Chemistry Research, Vol. 34, Issue 2 https://doi.org/10.1021/ie00041a012	journal	February 1995
The Chemical State of Gallium in Working Alkane Dehydrocyclodimerization Catalysts. In situ Gallium K-Edge X-Ray Absorption Spectroscopy Meitzner, G.; Iglesia, E.; Baumgartner, J. Journal of Catalysis, Vol. 140, Issue 1, p. 209-225 https://doi.org/10.1006/jcat.1993.1079	journal	March 1993
On two alternative mechanisms of ethane activation over ZSM-5 zeolite modified by Zn2+ and Ga1+ cations Kazansky, V. B.; Subbotina, I. R.; Rane, N. Physical Chemistry Chemical Physics, Vol. 7, Issue 16 https://doi.org/10.1039/b506782k	journal	January 2005
Correlations between Dispersion, Acidity, Reducibility, and Propane Aromatization Activity of Gallium Species Supported on HZSM5 Zeolites Rodrigues, Victor de O.; Eon, Jean-Guillaume; Faro, Arnaldo C. The Journal of Physical Chemistry C, Vol. 114, Issue 10 https://doi.org/10.1021/jp910642p	journal	March 2010
Characterization and reactivity of Ga+ and GaO+ cations in zeolite ZSM-5 Rane, N.; Overweg, A.; Kazansky, V. Journal of Catalysis, Vol. 239, Issue 2 https://doi.org/10.1016/j.jcat.2006.03.004	journal	April 2006
Organometallic model complexes elucidate the active gallium species in alkane dehydrogenation catalysts based on ligand effects in Ga K-edge XANES Getsoian, Andrew “Bean”; Das, Ujjal; Camacho-Bunquin, Jeffrey Catalysis Science & Technology, Vol. 6, Issue 16 https://doi.org/10.1039/C6CY00698A	journal	January 2016
A comprehensive density functional theory study of ethane dehydrogenation over reduced extra-framework gallium species in ZSM-5 zeolite Pidko, E.; Kazansky, V.; Hensen, E. Journal of Catalysis, Vol. 240, Issue 1 https://doi.org/10.1016/j.jcat.2006.03.011	journal	May 2006
A density functional study on the effect of the zeolite cavity on its catalytic activity: The dehydrogenation and cracking reactions of isobutane over HZSM-5 and HY zeolites Milas, Ivan; Chaer Nascimento, Marco Antonio Chemical Physics Letters, Vol. 418, Issue 4-6 https://doi.org/10.1016/j.cplett.2005.10.149	journal	February 2006
High ethane dehydrogenation activity of [GaH]2+Al pair sites in Ga/H-[Al]ZSM-5: A DFT thermochemical analysis of the catalytic sites under reaction conditions Joshi, Y.; Thomson, K. Journal of Catalysis, Vol. 246, Issue 2 https://doi.org/10.1016/j.jcat.2006.11.032	journal	March 2007
Dehydrogenation of Light Alkanes over Isolated Gallyl Ions in Ga/ZSM-5 Zeolites Pidko, Evgeny A.; Hensen, Emiel J. M.; van Santen, Rutger A. The Journal of Physical Chemistry C, Vol. 111, Issue 35 https://doi.org/10.1021/jp072110z	journal	September 2007
Quantum chemical calculation of the catalytic reaction of ethane dehydrogenation on gallium oxide-hydroxide binuclear clusters in oxidized GaO/ZSM-5 zeolite Kuz’min, I. V.; Zhidomirov, G. M.; Solkan, V. N. Kinetics and Catalysis, Vol. 50, Issue 5 https://doi.org/10.1134/S0023158409050188	journal	September 2009
Cluster Model DFT Study of CO Adsorption to Gallium Ions in Ga/HZSM-5 Zhidomirov, George M.; Shubin, Alexander A.; Milov, M. A. The Journal of Physical Chemistry C, Vol. 112, Issue 9 https://doi.org/10.1021/jp076379u	journal	March 2008
The roles of gallium hydride and Brønsted acidity in light alkane dehydrogenation mechanisms using Ga-exchanged HZSM-5 catalysts: A DFT pathway analysis Joshi, Yogesh V.; Thomson, Kendall T. Catalysis Today, Vol. 105, Issue 1 https://doi.org/10.1016/j.cattod.2005.04.017	journal	July 2005
Effect of the Zeolite Cavity on the Mechanism of Dehydrogenation of Light Alkanes over Gallium-Containing Zeolites Pereira, Marcio Soares; da Silva, Alexander Martins; Nascimento, Marco Antonio Chaer The Journal of Physical Chemistry C, Vol. 115, Issue 20, p. 10104-10113 https://doi.org/10.1021/jp201107x	journal	April 2011
Theoretical Study on the Dehydrogenation Reaction of Alkanes Catalyzed by Zeolites Containing Nonframework Gallium Species Pereira, Marcio Soares; Chaer Nascimento, Marco Antonio The Journal of Physical Chemistry B, Vol. 110, Issue 7 https://doi.org/10.1021/jp055104g	journal	February 2006
Ethane conversion: Kinetic evidence for the competition of consecutive steps for the same active centre Bandiera, Jean; Taârit, Younès Ben Applied Catalysis A: General, Vol. 152, Issue 1 https://doi.org/10.1016/S0926-860X(96)00345-6	journal	April 1997
Density functional theory studies of nitrous oxide adsorption and decomposition on Ga-ZSM-5 Solkan, V. N.; Zhidomirov, G. M.; Kazansky, V. B. International Journal of Quantum Chemistry, Vol. 107, Issue 13 https://doi.org/10.1002/qua.21375	journal	January 2007
Water-Promoted Hydrocarbon Activation Catalyzed by Binuclear Gallium Sites in ZSM-5 Zeolite Hensen, Emiel J. M.; Pidko, Evgeny A.; Rane, Neelesh Angewandte Chemie International Edition, Vol. 46, Issue 38 https://doi.org/10.1002/anie.200702463	journal	September 2007
Effects of pretreatments on state of gallium and aromatization activity of gallium/ZSM-5 catalysts Dooley, Kerry M.; Chang, Chauchyun; Price, Geoffrey L. Applied Catalysis A: General, Vol. 84, Issue 1 https://doi.org/10.1016/0926-860X(92)80336-B	journal	May 1992
Identity and chemical function of gallium species inferred from microkinetic modeling studies of propane aromatization over Ga/HZSM-5 catalysts Krishnamurthy, Gowri; Bhan, Aditya; Delgass, W. Nicholas Journal of Catalysis, Vol. 271, Issue 2 https://doi.org/10.1016/j.jcat.2010.02.026	journal	May 2010
Structure−Reactivity Relationship for Catalytic Activity of Gallium Oxide and Sulfide Clusters in Zeolite Pidko, Evgeny A.; van Santen, Rutger A. The Journal of Physical Chemistry C, Vol. 113, Issue 11 https://doi.org/10.1021/jp8113607	journal	February 2009
Self-organization of extraframework cations in zeolites Pidko, Evgeny A.; Hensen, Emiel J. M.; van Santen, Rutger A. Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 468, Issue 2143 https://doi.org/10.1098/rspa.2012.0057	journal	March 2012
Non-localized charge compensation in zeolites: A periodic DFT study of cationic gallium-oxide clusters in mordenite Pidko, E.; Hensen, E.; Zhidomirov, G. Journal of Catalysis, Vol. 255, Issue 2 https://doi.org/10.1016/j.jcat.2008.02.027	journal	April 2008
Multinuclear gallium-oxide cations in high-silica zeolites Pidko, Evgeny A.; van Santen, Rutger A.; Hensen, Emiel J. M. Physical Chemistry Chemical Physics, Vol. 11, Issue 16 https://doi.org/10.1039/b815943b	journal	January 2009
Ethylene adsorption and transformation on zeolite Ga+/ZSM-5 Kuz´min, I. V.; Sokolova, N. A.; Subbotina, I. R. Russian Chemical Bulletin, Vol. 64, Issue 2 https://doi.org/10.1007/s11172-015-0857-y	journal	February 2015
Adsorption properties of oxidized gallium-modified zeolite ZSM-5 from diffuse reflectance IR and quantum-chemical data: 1. Interaction with hydrogen and ethane Subbotina, I. R.; Sokolova, N. A.; Kuz’min, I. V. Kinetics and Catalysis, Vol. 48, Issue 5 https://doi.org/10.1134/S0023158407050199	journal	September 2007
Ab Initio and Density Functional Study of the Activation Barrier for Ethane Cracking in Cluster Models of Zeolite H-ZSM-5 Zygmunt, S. A.; Curtiss, L. A.; Zapol, P. The Journal of Physical Chemistry B, Vol. 104, Issue 9 https://doi.org/10.1021/jp993194h	journal	February 2000
Mechanisms of Hydrogen Exchange of Methane with H-Zeolite Y: An ab Initio Embedded Cluster Study Vollmer, James M.; Truong, Thanh N. The Journal of Physical Chemistry B, Vol. 104, Issue 26 https://doi.org/10.1021/jp0008445	journal	June 2000
Theoretical Investigation of Benzene Alkylation with Ethene over H-ZSM-5 Hansen, Niels; Brüggemann, Till; Bell, Alexis T. The Journal of Physical Chemistry C, Vol. 112, Issue 39 https://doi.org/10.1021/jp8036022	journal	September 2008
Impact of long-range electrostatic and dispersive interactions on theoretical predictions of adsorption and catalysis in zeolites Mansoor, Erum; Van der Mynsbrugge, Jeroen; Head-Gordon, Martin Catalysis Today, Vol. 312 https://doi.org/10.1016/j.cattod.2018.02.007	journal	August 2018
The Roles of Entropy and Enthalpy in Stabilizing Ion-Pairs at Transition States in Zeolite Acid Catalysis Gounder, Rajamani; Iglesia, Enrique Accounts of Chemical Research, Vol. 45, Issue 2 https://doi.org/10.1021/ar200138n	journal	August 2011
Improved Force-Field Parameters for QM/MM Simulations of the Energies of Adsorption for Molecules in Zeolites and a Free Rotor Correction to the Rigid Rotor Harmonic Oscillator Model for Adsorption Enthalpies Li, Yi-Pei; Gomes, Joseph; Mallikarjun Sharada, Shaama The Journal of Physical Chemistry C, Vol. 119, Issue 4 https://doi.org/10.1021/jp509921r	journal	January 2015
Theoretical Analysis of the Influence of Pore Geometry on Monomolecular Cracking and Dehydrogenation of n -Butane in Brønsted Acidic Zeolites Van der Mynsbrugge, Jeroen; Janda, Amber; Mallikarjun Sharada, Shaama ACS Catalysis, Vol. 7, Issue 4 https://doi.org/10.1021/acscatal.6b03646	journal	March 2017
Insights into the Kinetics of Cracking and Dehydrogenation Reactions of Light Alkanes in H-MFI Mallikarjun Sharada, Shaama; Zimmerman, Paul M.; Bell, Alexis T. The Journal of Physical Chemistry C, Vol. 117, Issue 24 https://doi.org/10.1021/jp402506m	journal	June 2013
Selection and Validation of Charge and Lennard-Jones Parameters for QM/MM Simulations of Hydrocarbon Interactions with Zeolites Zimmerman, Paul M.; Head-Gordon, Martin; Bell, Alexis T. Journal of Chemical Theory and Computation, Vol. 7, Issue 6 https://doi.org/10.1021/ct2001655	journal	May 2011
Computational Study of p -Xylene Synthesis from Ethylene and 2,5-Dimethylfuran Catalyzed by H-BEA Li, Yi-Pei; Head-Gordon, Martin; Bell, Alexis T. The Journal of Physical Chemistry C, Vol. 118, Issue 38 https://doi.org/10.1021/jp506664c	journal	September 2014
Crystal Structure of Dehydrated CsZSM-5 (5.8Al): Evidence for Nonrandom Aluminum Distribution ^† Olson, David H.; Khosrovani, Nazy; Peters, Alan W. The Journal of Physical Chemistry B, Vol. 104, Issue 20 https://doi.org/10.1021/jp000417r	journal	May 2000
Accurate Prediction of Hydrocarbon Interactions with Zeolites Utilizing Improved Exchange-Correlation Functionals and QM/MM Methods: Benchmark Calculations of Adsorption Enthalpies and Application to Ethene Methylation by Methanol Gomes, Joseph; Zimmerman, Paul M.; Head-Gordon, Martin The Journal of Physical Chemistry C, Vol. 116, Issue 29 https://doi.org/10.1021/jp303321s	journal	July 2012
Advances in methods and algorithms in a modern quantum chemistry program package Shao, Yihan; Molnar, Laszlo Fusti; Jung, Yousung Phys. Chem. Chem. Phys., Vol. 8, Issue 27 https://doi.org/10.1039/B517914A	journal	January 2006
Efficient exploration of reaction paths via a freezing string method Behn, Andrew; Zimmerman, Paul M.; Bell, Alexis T. The Journal of Chemical Physics, Vol. 135, Issue 22 https://doi.org/10.1063/1.3664901	journal	December 2011
Long-range corrected hybrid density functionals with damped atom–atom dispersion corrections Chai, Jeng-Da; Head-Gordon, Martin Physical Chemistry Chemical Physics, Vol. 10, Issue 44 https://doi.org/10.1039/b810189b	journal	January 2008
Thirty years of density functional theory in computational chemistry: an overview and extensive assessment of 200 density functionals Mardirossian, Narbe; Head-Gordon, Martin Molecular Physics, Vol. 115, Issue 19 https://doi.org/10.1080/00268976.2017.1333644	journal	April 2017
A look at the density functional theory zoo with the advanced GMTKN55 database for general main group thermochemistry, kinetics and noncovalent interactions Goerigk, Lars; Hansen, Andreas; Bauer, Christoph Physical Chemistry Chemical Physics, Vol. 19, Issue 48 https://doi.org/10.1039/C7CP04913G	journal	January 2017
Theoretical Study of 4-(Hydroxymethyl)benzoic Acid Synthesis from Ethylene and 5-(Hydroxymethyl)furoic Acid Catalyzed by Sn-BEA Li, Yi-Pei; Head-Gordon, Martin; Bell, Alexis T. ACS Catalysis, Vol. 6, Issue 8 https://doi.org/10.1021/acscatal.6b01160	journal	July 2016
Analysis of the Reaction Mechanism and Catalytic Activity of Metal-Substituted Beta Zeolite for the Isomerization of Glucose to Fructose Li, Yi-Pei; Head-Gordon, Martin; Bell, Alexis T. ACS Catalysis, Vol. 4, Issue 5 https://doi.org/10.1021/cs401054f	journal	April 2014
Natural bond Orbitals and Extensions of Localized Bonding Concepts Weinhold, Frank; Landis, Clark R. Chem. Educ. Res. Pract., Vol. 2, Issue 2 https://doi.org/10.1039/B1RP90011K	journal	January 2001
Advances in molecular quantum chemistry contained in the Q-Chem 4 program package Shao, Yihan; Gan, Zhengting; Epifanovsky, Evgeny Molecular Physics, Vol. 113, Issue 2 https://doi.org/10.1080/00268976.2014.952696	journal	September 2014
Normal Mode Analysis in Zeolites: Toward an Efficient Calculation of Adsorption Entropies De Moor, Bart A.; Ghysels, An; Reyniers, Marie-Françoise Journal of Chemical Theory and Computation, Vol. 7, Issue 4 https://doi.org/10.1021/ct1005505	journal	March 2011
Quantum Chemical Free Energies: Structure Optimization and Vibrational Frequencies in Normal Modes Piccini, GiovanniMaria; Sauer, Joachim Journal of Chemical Theory and Computation, Vol. 9, Issue 11 https://doi.org/10.1021/ct4005504	journal	October 2013
Supramolecular Binding Thermodynamics by Dispersion-Corrected Density Functional Theory Grimme, Stefan Chemistry - A European Journal, Vol. 18, Issue 32 https://doi.org/10.1002/chem.201200497	journal	July 2012
Adsorption Thermodynamics and Intrinsic Activation Parameters for Monomolecular Cracking of n -Alkanes on Brønsted Acid Sites in Zeolites Janda, Amber; Vlaisavljevich, Bess; Lin, Li-Chiang The Journal of Physical Chemistry C, Vol. 119, Issue 19 https://doi.org/10.1021/acs.jpcc.5b01715	journal	May 2015
A refinement of everyday thinking: the energetic span model for kinetic assessment of catalytic cycles: Energetic span, a refinement of everyday thinking Kozuch, Sebastian Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 5 https://doi.org/10.1002/wcms.1100	journal	April 2012
How to Conceptualize Catalytic Cycles? The Energetic Span Model Kozuch, Sebastian; Shaik, Sason Accounts of Chemical Research, Vol. 44, Issue 2 https://doi.org/10.1021/ar1000956	journal	February 2011
“Turning Over” Definitions in Catalytic Cycles Kozuch, Sebastian; Martin, Jan M. L. ACS Catalysis, Vol. 2, Issue 12 https://doi.org/10.1021/cs3005264	journal	November 2012
A Combined Kinetic−Quantum Mechanical Model for Assessment of Catalytic Cycles: Application to Cross-Coupling and Heck Reactions Kozuch, Sebastian; Shaik, Sason Journal of the American Chemical Society, Vol. 128, Issue 10 https://doi.org/10.1021/ja0559146	journal	March 2006
Activation of Small Alkanes in Ga-Exchanged Zeolites: A Quantum Chemical Study of Ethane Dehydrogenation Frash, M. V.; van Santen, R. A. The Journal of Physical Chemistry A, Vol. 104, Issue 11 https://doi.org/10.1021/jp993414r	journal	March 2000
On catalyst activation and reaction mechanisms in propane aromatization on Ga/HZSM5 catalysts Rodrigues, Victor de O.; Faro Júnior, Arnaldo C. Applied Catalysis A: General, Vol. 435-436 https://doi.org/10.1016/j.apcata.2012.05.036	journal	September 2012
The Nature of the Chemical Bond. iv. the Energy of Single Bonds and the Relative Electronegativity of Atoms Pauling, Linus Journal of the American Chemical Society, Vol. 54, Issue 9 https://doi.org/10.1021/ja01348a011	journal	September 1932
Effects of Si/Al Ratio on the Distribution of Framework Al and on the Rates of Alkane Monomolecular Cracking and Dehydrogenation in H-MFI Janda, Amber; Bell, Alexis T. Journal of the American Chemical Society, Vol. 135, Issue 51 https://doi.org/10.1021/ja4081937	journal	December 2013
Catalytic Consequences of Spatial Constraints and Acid Site Location for Monomolecular Alkane Activation on Zeolites Gounder, Rajamani; Iglesia, Enrique Journal of the American Chemical Society, Vol. 131, Issue 5 https://doi.org/10.1021/ja808292c	journal	February 2009
Different Efficiency of Zn ²⁺ and ZnO Species for Methane Activation on Zn-Modified Zeolite Gabrienko, Anton A.; Arzumanov, Sergei S.; Toktarev, Alexander V. ACS Catalysis, Vol. 7, Issue 3 https://doi.org/10.1021/acscatal.6b03036	journal	February 2017
Competitive pathways of methane activation on Zn ²⁺ -modified ZSM-5 zeolite: H/D hydrogen exchange with Brønsted acid sites versus dissociative adsorption to form Zn-methyl species Arzumanov, Sergei S.; Gabrienko, Anton A.; Freude, Dieter Catalysis Science & Technology, Vol. 6, Issue 16 https://doi.org/10.1039/C6CY00878J	journal	January 2016
Methane Activation on Zn ²⁺ -Exchanged ZSM-5 Zeolites. The Effect of Molecular Oxygen Addition Gabrienko, Anton A.; Arzumanov, Sergei S.; Luzgin, Mikhail V. The Journal of Physical Chemistry C, Vol. 119, Issue 44 https://doi.org/10.1021/acs.jpcc.5b08759	journal	October 2015
The “Alkyl” and “Carbenium” Pathways of Methane Activation on Ga-Modified Zeolite BEA: ¹³ C Solid-State NMR and GC-MS Study of Methane Aromatization in the Presence of Higher Alkane Luzgin, Mikhail V.; Gabrienko, Anton A.; Rogov, Vladimir A. The Journal of Physical Chemistry C, Vol. 114, Issue 49 https://doi.org/10.1021/jp1078899	journal	November 2010
Catalytic cracking, dehydrogenation, and aromatization of isobutane over Ga/HZSM-5 and Zn/HZSM-5 at low pressures Sun, Yanping; Brown, Trevor C. International Journal of Chemical Kinetics, Vol. 34, Issue 8 https://doi.org/10.1002/kin.10073	journal	January 2002
Lewis–Brønsted Acid Pairs in Ga/H-ZSM-5 To Catalyze Dehydrogenation of Light Alkanes Schreiber, Moritz W.; Plaisance, Craig P.; Baumgärtl, Martin Journal of the American Chemical Society, Vol. 140, Issue 14 https://doi.org/10.1021/jacs.7b12901	journal	February 2018

Cited By (1)

Quantification and Statistical Analysis of Errors Related to the Approximate Description of Active Site Models in Metal‐Exchanged Zeolites Thirumalai, Hari; Rimer, Jeffrey D.; Grabow, Lars C. ChemCatChem, Vol. 11, Issue 20 https://doi.org/10.1002/cctc.201901229	journal	September 2019

Similar Records

Mechanism and kinetics of light alkane dehydrogenation and cracking over isolated Ga species in Ga/H-MFI

Journal Article · Fri Feb 19 00:00:00 EST 2021 · ACS Catalysis · OSTI ID:1571106

Phadke, NM; Mansoor, E; Head-Gordon, M; +1 more

Mechanism and Kinetics of Propane Dehydrogenation and Cracking over Ga/H-MFI Prepared via Vapor-Phase Exchange of H-MFI with GaCl₃

Journal Article · Wed Dec 26 00:00:00 EST 2018 · Journal of the American Chemical Society · OSTI ID:1571106

Phadke, Neelay M.; Mansoor, Erum; Bondil, Matthieu; +2 more

Activation of small alkanes in Ga-exchanged zeolites: A quantum chemical study of ethane dehydrogenation

Journal Article · Thu Mar 23 00:00:00 EST 2000 · Journal of Physical Chemistry A: Molecules, Spectroscopy, Kinetics, Environment, amp General Theory · OSTI ID:1571106

Frash, M V; Santen, R.A. van

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
dehydrogenation
hydrides
molecular catalysis
zeolites
DFT
light alkanes
gallium

Title: Computational Modeling of the Nature and Role of Ga Species for Light Alkane Dehydrogenation Catalyzed by Ga/H-MFI

Citation Formats

References (70)

Cited By (1)

Similar Records

Related Subjects