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Record W2292460290

Molecular modeling of supported precious metal catalyst for the reduction of automobile exhaust : a quantum chemical molecular dynamics study

2011· dissertation· en· W2292460290 on OpenAlex

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.

Bibliographic record

VenueInstitutional Repositories DataBase (IRDB) · 2011
Typedissertation
Languageen
FieldMaterials Science
TopicCatalytic Processes in Materials Science
Canadian institutionsHatch (Canada)
Fundersnot available
KeywordsPrecious metalCatalysisQuantum chemicalMolecular dynamicsChemistryNanotechnologyMaterials scienceChemical engineeringProcess engineeringEngineeringOrganic chemistryComputational chemistryMolecule
DOInot available

Abstract

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Catalysis is enabling technology to promote sustainability, environmental consciousness, energy conservation, health and quality of life.Catalytic purification has proven to be an efficient way to reduce emissions from exhaust gases and the idea of the three-way catalyst (TWC) is to remove CO and NOx and to oxidize unburnt hydrocarbons.The goal of this research is to investigate insight of the most relevant mechanisms of supported noble meta l catalyst for the reduction of automobile exhaust, which will accelerate the speed of the development of highperformance catalysts by the physicochemical study.In this study I have applied ultra accelerated quantum chemical molecular dynamics (UA-QCMD) to investigate the reaction mechanism that occurs in TWC.As we know hydrogen spillover play a vital role in emerging technologies for the reduction of NO x in automobile exhausts.Besides this CO oxidation NO reduction reaction on small size Pd clusters supported on MgO(100) also has a wide range of application such as reduction of NO x .Considering the application of above two reactions, the present research investigate the reduction of NO x by two UA-QCMD simulations such as by (i) spillover hydrogen and (ii) CO oxidation NO reduction reaction on different supported precious metal catalysts.Supported noble metal catalysts such as Pt/-Al 2 O 3 , Pt/CeO 2 show special peculiarities on hydrogen adsorption, the extent of which is increased by hydrogen spillover.The direct observation of dissociative adsorption of hydrogen and diffusion of hydrogen on Pt/-Al 2 O 3 and Pt/CeO 2 catalyst surface were successfully investigated by UA-QCMD method.Here I have successfully investigated the mechanism of hydrogen spillover reaction and unveiled the factors that involved in this chemical transformation by UA-QCMD method.Hydrogen spillovers in gas phase were simulated at the first time on Pt/-Al 2 O 3 and Pt/CeO 2 catalyst surface.Moreover, this study indicates that the CeO 2 support has strong interaction with Pt catalyst, which may cause an increase in metal support interaction, Pt activity and enhancement of the metal catalyst dispersions.However, Pt/-Al 2 O 3 catalyst, compared with Pt/CeO 2 , provides a clear manifestation of the role of the metal-support interaction in modifying the catalytic behavior of the metal.As we know hydrogen spillover reaction consists of several elementary steps o f reactions such as dissociation, adsorption, diffusion and desorption.Among these steps frequent dissociative adsorption of hydrogen on the metal surface is important for hydrogen spillover.But the dissociation of hydrogen depends on coverage of the surface.Since no studies to date have been able to study the spillover step in isolation, all the studies interpret experimental data for a combination of sequential steps.Here influences of surface hydrogen vacancy for the dissociative adsorption of hydrogen on different metal surfaces were investigated.MD simulation together with electronic structure calculation shows that di-vacancy is sufficient for the dissociative adsorption of hydrogen on Pd (100) surface; in contrast at least tri-vacancy is required for Pd (111) surface.It was found that fully hydrogen covered step sites can dissociate hydrogen moderately and that a monovacancy site is suitable for significant dissociation of hydrogen.However, in terrace sites of the Pd (332) surface, it was observed that hydrogen dissociation takes place only at the Pd sites where the metal atom is not bound to any preadsorbed H atom.CO oxidation and NO reduction reaction on supported precious metal catalyst were investigated by quantum chemical molecular dynamics method.Here catalyst aids the reaction of the CO with the remaining oxygen in the exhaust gas.Here the pathways and energetic of the involved elementary reactions under different catalytic conditions were investigated.

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Full frame distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.001
metaresearch head score (Gemma)0.001
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow)
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.026
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.000
Science and technology studies0.0000.001
Scholarly communication0.0000.001
Open science0.0010.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0000.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.019
GPT teacher head0.286
Teacher spread0.267 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it