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Record W4392375236 · doi:10.26434/chemrxiv-2024-r67fv

Vendor-dependent mobile phase contaminants affect neutral lipid analysis in lipidomics protocols

2024· preprint· en· W4392375236 on OpenAlexafffund
Joshua Roberts, Angela S. Radnoff, Aleksandra Bushueva, J. Ménard, Karl V. Wasslen, Meaghan Harley, Jeffrey M. Manthorpe, Jeffrey C. Smith

Bibliographic record

VenueChemRxiv · 2024
Typepreprint
Languageen
FieldBiochemistry, Genetics and Molecular Biology
TopicMetabolomics and Mass Spectrometry Studies
Canadian institutionsCarleton University
FundersNatural Sciences and Engineering Research Council of CanadaGovernment of OntarioCanada Foundation for InnovationOntario Research FoundationCarleton University
KeywordsLipidomicsChemistryAdductChromatographyMass spectrometryMethanolAlkylLiquid chromatography–mass spectrometryOrganic chemistryBiochemistry

Abstract

fetched live from OpenAlex

Lipidomics is a well-established field, enabled by modern liquid chromatography mass spectrometry (LCMS) technology, rapidly generating large amounts of data. Lipid extracts derived from biological samples are complex and most spectral features in LCMS lipidomics datasets remain unidentified, colloquially termed lipidomics “dark matter”. In-depth analyses of triacylglycerol, diacylglycerol, and cholesterol ester species revealed the expected ammoniated and sodiated ions as well as 5 additional higher mass dark matter peaks. These additional peaks were of relatively high intensity and resulted from analyte adduction with alkylated amine contaminants from LCMS-grade methanol and isopropanol. Tandem MS (MS/MS) of adduct peaks yielded no lipid structural information, producing only an intense ion of the adducted contaminant. Analysis of bovine liver extract identified 33 neutral lipids with an additional 73 alkyl amine adducts. Removing alcohols in place for acetonitrile and methyl tert-butyl ether in the mobile phase resulted in a 60% decrease in neutral lipid annotations, but eliminated the formation of alkyl amine adducts. Analysis of LCMS-grade methanol and isopropanol from different vendors revealed alkyl amine adduct formation in one out of three different brands that were tested. Substituting solvents increased lipid annotations by 36.5% or 27.4%, depending on the vendor and resulted in >2.5-fold increases in peak area for neutral lipid species, dramatically affecting their quantification and detection. Using principal component analysis, the same bovine liver sample separated into vendor-based clusters. These findings demonstrate the importance of solvent selection and disclosure during lipidomics protocols and highlight the challenges when comparing data between experiments.

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)0.009
metaresearch head score (Gemma)0.013
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: none
Teacher disagreement score0.009
Threshold uncertainty score0.048

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0090.013
Meta-epidemiology (narrow)0.0020.002
Meta-epidemiology (broad)0.0010.001
Bibliometrics0.0020.002
Science and technology studies0.0020.001
Scholarly communication0.0020.002
Open science0.0020.003
Research integrity0.0020.003
Insufficient payload (model declined to judge)0.0060.010

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 head0.019
GPT teacher head0.335
Teacher spread0.315 · 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

Citations1
Published2024
Admission routes2
Has abstractyes

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