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Record W2140488270 · doi:10.1021/om040005v

Zeolite Activation of Organometallics:  Anchoring and Decarbonylation Kinetics of Mo(CO)<sub>6</sub> in Dehydrated Na<sub>56</sub>Y Zeolite

2004· article· en· W2140488270 on OpenAlexaff
Anthony L. Fernandez, Jianbin Hao, Roberta L. Parkes, Anthony J. Poë, Eduardo J. S. Vichi

Bibliographic record

VenueOrganometallics · 2004
Typearticle
Languageen
FieldChemistry
TopicZeolite Catalysis and Synthesis
Canadian institutionsUniversity of Toronto
Fundersnot available
KeywordsDecarbonylationChemistryInfrared spectroscopyZeolitePhysical chemistryCatalysisPhotochemistryMedicinal chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Quantitative temperature-dependent kinetic studies are reported of thermal reactions of Mo(CO) 6 that has been newly encapsulated in the α-cages of a Na 56 Y zeolite host. Under static vacuum, Mo(CO) 6 undergoes parallel anchoring and decarbonylation reactions, the latter yielding (OC) 3 Mo−Na 56 Y directly and the former resulting in the development of a characteristic six-band spectrum in the C−O stretching region. Kinetic and spectroscopic evidence was obtained for there being two different forms of (OC) 3 Mo−Na 56 Y. The activation parameters are unusual, with very low enthalpies and extremely negative entropies, viz. Δ H ⧧ = 40 ± 3 kJ mol - 1 and Δ S ⧧ = −185 ± 9 J K - 1 mol - 1 for anchoring and decarbonylation. This contrasts with the typically high enthalpic and positive entropic factors reported for corresponding CO dissociative reactions in xylene (Δ H ⧧ = 133 ± 6 kJ mol - 1 and Δ S ⧧ = +28 ± 16 J K - 1 mol - 1 ) or even the quite unusual values Δ H ⧧ = 61 ± 5 kJ mol - 1 and Δ S ⧧ = −139 ± 13 J K - 1 mol - 1 reported previously for 13 CO exchange in Mo(CO) 6 −Na 56 Y. It is concluded that the inner surface of Na 56 Y provides different activating environments for different reactions, behaving as multidentate anionic “zeolate” nucleophiles, with varying numbers of O 2 - ions participating in highly ordered transition states. A common intermediate, with three O 2 - ions participating in the anchoring and decarbonylation process, is proposed, one with two O 2 - ions being proposed for the 13 CO exchange reaction. The importance of temperature-dependent time-resolved infrared spectroscopy in elucidating such intimate mechanistic details is emphasized.

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)0.000
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 score0.009
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0010.001
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0010.002
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
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 head0.012
GPT teacher head0.216
Teacher spread0.205 · 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.

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

Citations6
Published2004
Admission routes1
Has abstractyes

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