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Record W3022569642 · doi:10.1039/d0cp01284j

The mechanism and ligand effects of single atom rhodium supported on ZSM-5 for the selective oxidation of methane to methanol

2020· article· en· W3022569642 on OpenAlexfundno aff
Rhys J. Bunting, Jillian M. Thompson, P. Hu

Bibliographic record

VenuePhysical Chemistry Chemical Physics · 2020
Typearticle
Languageen
FieldMaterials Science
TopicCatalytic Processes in Materials Science
Canadian institutionsnot available
FundersEngineering and Physical Sciences Research CouncilQueen's UniversityQueen's University Belfast
KeywordsRhodiumMethanolMethaneChemistryPartial oxidationLigand (biochemistry)ZSM-5Atom (system on chip)Anaerobic oxidation of methanePhotochemistryCatalysisZeoliteOrganic chemistry

Abstract

fetched live from OpenAlex

The mechanism for the partial oxidation of methane to methanol on single atom rhodium supported on ZSM-5 is investigated by DFT. The most favoured mechanism for methane activation is shown to be via oxidative addition at an undercoordinated rhodium metal centre and not through a typical metal oxo intermediate. The formation of a C-OH bond, and not methane activation, is found to be the rate determining step. CO coordinated to the rhodium centre is observed to strongly promote this bond formation. Water is required in the system to help prevent catalyst poisoning by CO, which greatly hinders the methane activation step, and to protonate an intermediate RhOOH species. These results suggest that more focus is required on methyl-oxygen bond formation and that exclusive consideration of methane activation will not completely explain some methane partial oxidation systems.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

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)0.000
metaresearch head score (Gemma)0.001
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesnone
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 score0.020
Threshold uncertainty score0.499

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
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 head0.015
GPT teacher head0.258
Teacher spread0.244 · 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

Classification

machine, unvalidated

Machine predicted; a candidate call from one teacher head, not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations33
Published2020
Admission routes1
Has abstractyes

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