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Record W4395007242 · doi:10.1002/chem.202400916

Thermal Equilibrium Between Quinoid/Biradical Forms Enhancing Electrochemical Amphotericity

2024· article· en· W4395007242 on OpenAlexaff
Yusuke Ishigaki, Shin‐ichi Mizuno, Kazuma Sugawara, Takumi Hashimoto, Shuichi Suzuki, Takanori Suzuki

Bibliographic record

VenueChemistry - A European Journal · 2024
Typearticle
Languageen
FieldChemistry
TopicPhotochemistry and Electron Transfer Studies
Canadian institutionsScience North
FundersPrecursory Research for Embryonic Science and TechnologyJapan Society for the Promotion of ScienceMinistry of Education, Culture, Sports, Science and Technology
KeywordsAnnulationThermalHydrocarbonElectrochemistryResonance (particle physics)ChemistryComputational chemistryPhotochemistryChemical physicsOrganic chemistryCatalysisPhysical chemistryThermodynamicsAtomic physicsPhysicsElectrode

Abstract

fetched live from OpenAlex

Abstract Upon dibenzo annulation on Thiele's hydrocarbon (tetraphenyl‐ p ‐quinodimethane), the quinoid form and the biradical form adopt quite different geometries, and thus are no longer resonance structures. When these two forms can interconvert rapidly due to the small energy barrier (Δ G ≠ ), the equilibrated mixture contains both forms in a ratio that is determined by the energy difference (Δ G o ) between the two forms. For a series of tetrakis[5‐(4‐methoxyphenyl)‐2‐thienyl]‐substituted derivatives, the more stable quinoid form and the metastable biradical form coexist in solution as an equilibrated mixture due to small Δ G ≠ (<15 kcal mol −1 ) and Δ G o (1–4 kcal mol −1 ), in which the proportion of the two forms can be regulated by temperature. Since the biradical form can undergo easy two‐electron (2e) oxidation to the corresponding dications as well as easy 2e‐reduction to the dianions, it exhibits very high electrochemical amphotericity. This character with a record‐small span for not only the first oxidation and reduction potentials but also the second those, [ E 1 sum ≈ E 2 sum = E 2 ox − E 2 red =ca. 1.4 V], is attained through thermally enhanced conversion to the biradical form from the corresponding quinoid form, the latter of which is less amphoteric due to higher E ox and lower E red values.

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)0.001
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow), Research integrity, Insufficient payload (model declined to judge)
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 score0.035
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
Meta-epidemiology (narrow)0.0010.001
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0010.000
Open science0.0010.000
Research integrity0.0000.002
Insufficient payload (model declined to judge)0.0020.000

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 head0.231
Teacher spread0.219 · 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

Citations8
Published2024
Admission routes1
Has abstractyes

Explore more

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