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Record W1996714169 · doi:10.1021/jp035677y

Ab Initio Study of the Deamination of Formamidine

2003· article· en· W1996714169 on OpenAlex
Christopher G. Flinn, Raymond A. Poirier, W. Andrzej Sokalski

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.
fundA Canadian funder is recorded on the work.

Bibliographic record

VenueThe Journal of Physical Chemistry A · 2003
Typearticle
Languageen
FieldChemistry
TopicChemical Reaction Mechanisms
Canadian institutionsMemorial University of Newfoundland
FundersNatural Sciences and Engineering Research Council of Canada
KeywordsChemistryDeaminationTransition stateDissociation (chemistry)Tetrahedral carbonyl addition compoundProtonationDensity functional theoryAb initioFormamideComputational chemistryTautomerKinetic isotope effectPhysical chemistryCrystallographyStereochemistryDeuteriumCatalysisOrganic chemistryIonAtomic physics

Abstract

fetched live from OpenAlex

The mechanism for the deamination of formamidine with OH -, H 2 O, and H 3 O + was investigated using computational techniques. Optimized geometries for reactants, intermediates, products, and transition states were determined at the RHF/6-31G(d) and MP2/6-31G(d) levels of theory. Single-point energies were determined at G1 and G2 and using density functional theory (B3LYP) at both optimized geometries and the 6-311G(d,p), 6-311+G(d,p), 6-311++G(d,p) (with OH - only), 6-311G(2df,p), and 6-311+G(3df,2p) basis sets. Frequencies were calculated for all structures studied at both geometries. Intrinsic reaction coordinate analysis was carried out for all transition states. Activation energies were calculated for each pathway investigated. Deamination with H 3 O + involves the formation of the same tetrahedral intermediate from the addition of water to either possible protonated formamidine cation followed by a 1,3-proton shift and dissociation to products. Deamination is an unlikely event because of the high activation-energy barrier to the formation of the intermediate (242.4 kJ mol -1 for pathway A and 243.5 kJ mol -1 for pathway B using G2 data). Two pathways for deamination with H 2 O were studied. Pathway A produced a tetrahedral intermediate by the addition of water followed by a 1,3-proton shift and dissociation to products, and pathway B involved the formation of the tautomer of the formamide product by reaction with water followed by a 1,3-proton shift to yield formamide. Deamination by either pathway is unlikely because of the high activation-energy barriers involved (212.7 kJ mol -1 for the formation of the tetrahedral intermediate of pathway A and 249.2 kJ mol -1 for the formation of the formamide tautomer of pathway B using G2 data). Deamination with OH - yields a tetrahedral intermediate with a much lower activation-energy barrier than for the reaction with H 3 O + and H 2 O (58.2 kJ mol -1 using G2 data), but the deprotonation of formamidine by hydroxide appears to be the most likely process because of the resonance-stabilized deprotonated formamidine anion/water complex formed (Δ E = −163.2 kJ mol -1 ).

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.

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 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 score0.008
Threshold uncertainty score0.263

Codex and Gemma teacher scores by category

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)0.0000.000

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 head0.013
GPT teacher head0.250
Teacher spread0.238 · 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