Molybdenum Carbide Nanocatalysts at Work in the in Situ Environment: A Density Functional Tight-Binding and Quantum Mechanical/Molecular Mechanical Study.
Heterogeneous reactions catalyzed by transition-metal-containing nanoparticles represent a crucial type of reaction in chemical industry. Because of the existing gap in understanding heterogeneous catalysis between a cluster of a few atoms and a bulk model of periodic slabs, reactions catalyzed by t...
| Publicado en: | Journal of the American Chemical Society Vol. 137; no. 12; pp. 4249 - 4260 |
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| Autores principales: | , |
| Formato: | Artículo |
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American Chemical Society
4/1/2015
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| Acceso en línea: | Ver este registro en EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=102925234&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 102925234 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 4/1/2015 vid: 137 iid: 12 pid: 997 pub: American Chemical Society artinfo: ui: 102925234 10.1021/jacs.5b01494 ppf: 4249 ppct: 11 formats: tig: atl: Molybdenum Carbide Nanocatalysts at Work in the in Situ Environment: A Density Functional Tight-Binding and Quantum Mechanical/Molecular Mechanical Study. aug: au: Xingchen Liu Salahub, Dennis R. affil: Department of Chemistry, Institute for Quantum Science and Technology, and Centre for Molecular Simulation, University of Calgary, 2500 University Drive NW, Calgary, Alberta T2N 1N4, Canada su: Catalysts Transition metals Nanoparticles Chemical industry Free energy (Thermodynamics) sug: subj: Catalysts Transition metals Nanoparticles Chemical industry Free energy (Thermodynamics) ab: Heterogeneous reactions catalyzed by transition-metal-containing nanoparticles represent a crucial type of reaction in chemical industry. Because of the existing gap in understanding heterogeneous catalysis between a cluster of a few atoms and a bulk model of periodic slabs, reactions catalyzed by transition-metal-containing nanoparticles are still not well understood. Herein, we provide a multiscale modeling approach to study the benzene hydrogenation reactions on molybdenum carbide nanoparticles (MCNPs) in the process of in situ heavy oil upgrading. By coupling the quantum mechanical (QM) density functional tight-binding (DFTB) method with a molecular mechanical (MM) force field, a QM/MM model was built to describe the reactants, the nanoparticles and the surroundings. Umbrella sampling (US) was used to calculate the free energy profiles of the benzene hydrogenation reactions in a model aromatic solvent in the in situ heavy oil upgrading conditions. By comparing with the traditional method in computational heterogeneous catalysis, the results reveal new features of the metallic MCNPs. Rather than being rigid, they are very flexible under working condition due to the entropic contributions of the MCNPs and the solvent, which greatly affect the free energy profiles of these nanoscale heterogeneous reactions. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2015 holdings: @attributes: islocal: N |
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