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Record W4385514138 · doi:10.1021/acs.analchem.3c01362

Application of <sup>15</sup>N-Edited <sup>1</sup>H–<sup>13</sup>C Correlation NMR Spectroscopy─Toward Fragment-Based Metabolite Identification and Screening via HCN Constructs

2023· article· en· W4385514138 on OpenAlexafffund
Daniel H. Lysak, William W. Wolff, Ronald Soong, Wolfgang Bermel, Ēriks Kupče, Amy Jenne, Rajshree Ghosh Biswas, Daniel Lane, Geneviève M. C. Gasmi-Seabrook, André J. Simpson

Bibliographic record

VenueAnalytical Chemistry · 2023
Typearticle
Languageen
FieldBiochemistry, Genetics and Molecular Biology
TopicMetabolomics and Mass Spectrometry Studies
Canadian institutionsPrincess Margaret Cancer CentreThe Scarborough HospitalUniversity of Toronto
FundersOntario Ministry of Research and InnovationNatural Sciences and Engineering Research Council of CanadaKrembil FoundationCanada Foundation for InnovationGovernment of Ontario
KeywordsHeteronuclear single quantum coherence spectroscopyChemistryHeteronuclear moleculeMetaboliteTwo-dimensional nuclear magnetic resonance spectroscopyMetabolomicsNuclear magnetic resonance spectroscopyChemical shiftCarbon-13 NMRNMR spectra databaseNuclear magnetic resonanceStereochemistrySpectral lineChromatographyBiochemistryPhysical chemistry

Abstract

fetched live from OpenAlex

Many key building blocks of life contain nitrogen moieties. Despite the prevalence of nitrogen-containing metabolites in nature, 15 N nuclei are seldom used in NMR-based metabolite assignment due to their low natural abundance and lack of comprehensive chemical shift databases. However, with advancements in isotope labeling strategies, 13 C and 15 N enriched metabolites are becoming more common in metabolomic studies. Simple multidimensional nuclear magnetic resonance (NMR) experiments that correlate 1 H and 15 N via single bond 1 J NH or multiple bond 2–3 J NH couplings using heteronuclear single quantum coherence (HSQC) or heteronuclear multiple bond coherence are well established and routinely applied for structure elucidation. However, a 1 H– 15 N correlation spectrum of a metabolite mixture can be difficult to deconvolute, due to the lack of a 15 N specific database. In order to bridge this gap, we present here a broadband 15 N-edited 1 H– 13 C HSQC NMR experiment that targets metabolites containing 15 N moieties. Through this approach, nitrogen-containing metabolites, such as amino acids, nucleotide bases, and nucleosides, are identified based on their 13 C, 1 H, and 15 N chemical shift information. This approach was tested and validated using a [ 15 N, 13 C] enriched Daphnia magna (water flea) metabolite extract, where the number of clearly resolved 15 N-containing peaks increased from only 11 in a standard HSQC to 51 in the 15 N-edited HSQC, and the number of obscured peaks decreased from 59 to just 7. The approach complements the current repertoire of NMR techniques for mixture deconvolution and holds considerable potential for targeted metabolite NMR in 15 N, 13 C enriched systems.

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 score0.002

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 integrity0.0000.001
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 head0.010
GPT teacher head0.253
Teacher spread0.243 · 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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