Ab Initio Investigation of CH4 Dehydrogenation on a (CeO2)10 ClusterClick to copy article linkArticle link copied!
- Carina S. T. PeraçaCarina S. T. PeraçaSão Carlos Institute of Chemistry, University of São Paulo, P.O. Box 780, 13560-970, São Carlos, SP, BrazilDepartment of Physics, Federal University of Pelotas, P.O. Box 354, 96010-900, Pelotas, RS, BrazilMore by Carina S. T. Peraça
- Karla F. AndrianiKarla F. AndrianiDepartment of Biological Sciences, Federal University of Piauí, P.O. Box 64900-000, 64900-000 Bom Jesus, PI, BrazilSão Carlos Institute of Chemistry, University of São Paulo, P.O. Box 780, 13560-970, São Carlos, SP, BrazilMore by Karla F. Andriani
- Maurício J. PiotrowskiMaurício J. PiotrowskiDepartment of Physics, Federal University of Pelotas, P.O. Box 354, 96010-900, Pelotas, RS, BrazilMore by Maurício J. Piotrowski
- Juarez L. F. Da Silva*Juarez L. F. Da Silva*Email: [email protected]São Carlos Institute of Chemistry, University of São Paulo, P.O. Box 780, 13560-970, São Carlos, SP, BrazilMore by Juarez L. F. Da Silva
Abstract
We report a theoretical investigation of the activation and dehydrogenation of CH4 on a (CeO2)10 cluster based on density functional theory calculations combined with the unity bond index-quadratic exponential potential approach. As expected, we identified a physisorption interaction mechanism between the CH4 and (CeO2)10 systems. Along the dehydrogenation, the interaction CHn–(CeO2)10 occurs by chemisorption via the formation of C–O and H–O bonds. Due to adsorption effects, the oxidation state of Ce atoms changes from Ce4+ to Ce3+, which results in the elongation of the Ce–O bonds due to the larger radius of the Ce3+ species, and hence, it affects the formation of the CO and CH3OH species. Our combined approach showed that the first dehydrogenation step involves a transition-state formation induced by the molecular hybridization before the CH3 radical formation. Finally, our results indicate trends for new compound formation, once the energy barrier involved in the first step of dehydrogenation is overcome.
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This article is cited by 4 publications.
- Daiki Takahashi, Akira Yoko, Gimyeong Seong, Kazuyuki Iwase, Tadafumi Adschiri, Takaaki Tomai. Degradation Behavior of CeO2-Based Nanoparticles as Oxygen Carriers for the Chemical Looping Process. ACS Applied Nano Materials 2025, 8
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- Pedro Ivo R. Moraes, Albert F. B. Bittencourt, Karla F. Andriani, Juarez L. F. Da Silva. Theoretical Insights into Methane Activation on Transition-Metal Single-Atom Catalysts Supported on the CeO2(111) Surface. The Journal of Physical Chemistry C 2023, 127
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, 16357-16366. https://doi.org/10.1021/acs.jpcc.3c02653
- Pedro Ivo R. Moraes, Carina S.T. Peraça, Juarez L.F. Da Silva. Single-atom catalysts on ceria substrates: Exploring cluster and surface effects on methane activation. Molecular Catalysis 2024, 564 , 114318. https://doi.org/10.1016/j.mcat.2024.114318
- Carina S. T. Peraça, Albert F. B. Bittencourt, Raquel C. Bezerra, Juarez L. F. Da Silva. Atomistic insights from DFT calculations into the catalytic properties on ceria-lanthanum clusters for methane activation. The Journal of Chemical Physics 2024, 160
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https://doi.org/10.1063/5.0198986
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