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Record W4313560101 · doi:10.1002/jms.4901

Probing the pyrolysis of ethyl formate in the dilute gas phase by synchrotron radiation and theory

2023· article· en· W4313560101 on OpenAlexafffund
Bethany Lowe, Alejandro L. Cardona, Juana Salas, András Bödi, P. Mayer, Maxi A. Burgos Paci

Bibliographic record

VenueJournal of Mass Spectrometry · 2023
Typearticle
Languageen
FieldEarth and Planetary Sciences
TopicAtmospheric chemistry and aerosols
Canadian institutionsUniversity of Ottawa
FundersNatural Sciences and Engineering Research Council of CanadaSecretaria de Ciencia y Tecnología - Universidad Nacional de CórdobaMinisterio de Ciencia, Tecnología e Innovación ProductivaConsejo Nacional de Investigaciones Científicas y TécnicasCompute Canada
KeywordsChemistryPhotoionizationPhotochemistryEthyl formateMethyl formatePyrolysisAnalytical Chemistry (journal)FormatePhysical chemistryIonIonizationOrganic chemistryMethanolCatalysis

Abstract

fetched live from OpenAlex

Abstract The thermal decomposition of the atmospheric constituent ethyl formate was studied by coupling flash pyrolysis with imaging photoelectron photoion coincidence (iPEPICO) spectroscopy using synchrotron vacuum ultraviolet (VUV) radiation at the Swiss Light Source (SLS). iPEPICO allows photoion mass‐selected threshold photoelectron spectra (ms‐TPES) to be obtained for pyrolysis products. By threshold photoionization and ion imaging, parent ions of neutral pyrolysis products and dissociative photoionization products could be distinguished, and multiple spectral carriers could be identified in several ms‐TPES. The TPES and mass‐selected TPES for ethyl formate are reported for the first time and appear to correspond to ionization of the lowest energy conformer having a cis (eclipsed) configuration of the O=C(H)–O–C(H2)–CH3 and trans (staggered) configuration of the O=C(H)–O–C(H2)–CH3 dihedral angles. We observed the following ethyl formate pyrolysis products: CH3CH2OH, CH3CHO, C2H6, C2H4, HC(O)OH, CH2O, CO2, and CO, with HC(O)OH and C2H4 pyrolyzing further, forming CO + H2O and C2H2 + H2. The reaction paths and energetics leading to these products, together with the products of two homolytic bond cleavage reactions, CH3CH2O + CHO and CH3CH2 + HC(O)O, were studied computationally at the M06‐2X‐GD3/aug‐cc‐pVTZ and SVECV‐f12 levels of theory, complemented by further theoretical methods for comparison. The calculated reaction pathways were used to derive Arrhenius parameters for each reaction. The reaction rate constants and branching ratios are discussed in terms of the residence time and newly suggest carbon monoxide as a competitive primary fragmentation product at high temperatures.

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 machine prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: metacan-v3-hybrid-931329e0061cValidation 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 score0.001
Threshold uncertainty score0.004

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
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 science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0010.000

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 head0.008
GPT teacher head0.228
Teacher spread0.220 · 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 source (direct Gemma or distilled Codex), 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

Citations6
Published2023
Admission routes2
Has abstractyes

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