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Record W4378470199 · doi:10.1021/jacs.3c02222

Chemical Reaction Networks Explain Gas Evolution Mechanisms in Mg-Ion Batteries

2023· article· en· W4378470199 on OpenAlexfundno aff
Evan Walter Clark Spotte‐Smith, Samuel M. Blau, Daniel Barter, Noel J. Leon, Nathan Hahn, Nikita S. Redkar, Kevin R. Zavadil, Chen Liao, Kristin A. Persson

Bibliographic record

VenueJournal of the American Chemical Society · 2023
Typearticle
Languageen
FieldEngineering
TopicAdvanced battery technologies research
Canadian institutionsnot available
FundersLawrence Berkeley National LaboratoryVehicle Technologies ProgramNational Renewable Energy LaboratoryNational Nuclear Security AdministrationOffice of ScienceSandia National LaboratoriesU.S. Department of EnergyPhilomathia FoundationBasic Energy SciencesNational Energy Research Scientific Computing Center
KeywordsChemistryElectrolyteElectrochemistryDiglymePassivationBattery (electricity)Reactivity (psychology)DecompositionDensity functional theoryReaction mechanismElectrodeChemical decompositionIonChemical reactionInorganic chemistryComputational chemistryPhysical chemistryThermodynamicsOrganic chemistryCatalysis

Abstract

fetched live from OpenAlex

High Resolution Image Download MS PowerPoint Slide Out-of-equilibrium electrochemical reaction mechanisms are notoriously difficult to characterize. However, such reactions are critical for a range of technological applications. For instance, in metal-ion batteries, spontaneous electrolyte degradation controls electrode passivation and battery cycle life. Here, to improve our ability to elucidate electrochemical reactivity, we for the first time combine computational chemical reaction network (CRN) analysis based on density functional theory (DFT) and differential electrochemical mass spectroscopy (DEMS) to study gas evolution from a model Mg-ion battery electrolyte─magnesium bistriflimide (Mg(TFSI) 2 ) dissolved in diglyme (G2). Automated CRN analysis allows for the facile interpretation of DEMS data, revealing H 2 O, C 2 H 4, and CH 3 OH as major products of G2 decomposition. These findings are further explained by identifying elementary mechanisms using DFT. While TFSI – is reactive at Mg electrodes, we find that it does not meaningfully contribute to gas evolution. The combined theoretical–experimental approach developed here provides a means to effectively predict electrolyte decomposition products and pathways when initially unknown.

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: Simulation or modeling · Consensus signal: Simulation or modeling
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.002
Threshold uncertainty score0.006

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 communication0.0000.001
Open science0.0010.000
Research integrity0.0000.000
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 head0.011
GPT teacher head0.253
Teacher spread0.242 · 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 designSimulation or modeling
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

Citations41
Published2023
Admission routes1
Has abstractyes

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