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Record W2082667783 · doi:10.1139/v01-120

<sup>1</sup>H NMR studies of proton transfer equilibria in hydrogen bonds the role of the entropy

2001· article· en· W2082667783 on OpenAlexvenueno aff
Roland Langner, Georg Zuńdel

Bibliographic record

VenueCanadian Journal of Chemistry · 2001
Typearticle
Languageen
FieldChemistry
TopicCrystallography and molecular interactions
Canadian institutionsnot available
Fundersnot available
KeywordsChemistryHydrogen bondProtonProtonationProton NMRCrystallographyAcceptorChemical shiftDeprotonationStereochemistryMoleculePhysical chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

The influence of the entropy on the proton transfer equilibria AH···B [Formula: see text]A–···H+B in the dimethylphosphinic acid (DMP)-N-base and in the methanesulfonic acid (MSA)-N-oxide hydrogen bonds is studied by 1H NMR spectroscopy as a function of the ΔpKa, i.e., the pKa of the base minus the pKa of the acid. It is shown that with increasing ΔpKa the proton transfers to the N-oxide acceptor. In the DMP + N-base family of systems, first the double-minimum proton potentials (ΔH = 0) occurs and only with further increasing ΔpKa do the POH···N [Formula: see text] PO–···H+N equilibria become symmetrical (ΔG = 0). ΔG and ΔH are connected by the Gibbs–Helmholtz equation, ΔG = ΔH –TΔS. Hence, the reason of this effect is the large negative interaction entropy term (ΔSI) arising from the large order around the polar structure, which shifts the equilibria strongly to the left-hand side. With the MSA-N-oxide hydrogen bonds a single-minimum proton potential was found. The minimum shifts with increasing ΔpKa from the donor to the acceptor of the O···H+···N hydrogen bonds. It is shown that with increasing ΔpKa the proton potential becomes on average symmetrical, whereas the proton is still largely on the left-hand side. This result is also explained by the large negative interaction entropy due to the order of the environment if the proton is at the acceptor B.Key words: entropy, hydrogen bonds, infrared, spectroscopy, proton transfer.

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)0.001
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 score0.003
Threshold uncertainty score0.011

Distilled classifier scores by category (both heads)

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 science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0030.000

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 head0.010
GPT teacher head0.227
Teacher spread0.217 · 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

Citations3
Published2001
Admission routes1
Has abstractyes

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