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Record W4399305702 · doi:10.1021/jacs.4c01353

Pourbaix Machine Learning Framework Identifies Acidic Water Oxidation Catalysts Exhibiting Suppressed Ruthenium Dissolution

2024· article· en· W4399305702 on OpenAlexafffund
Jehad Abed, Javier Heras‐Domingo, Rohan Yuri Sanspeur, Mingchuan Luo, Wajdi Alnoush, Debora Meira, Hsiao‐Tsu Wang, Jian Wang, Jigang Zhou, Daojin Zhou, Khalid Fatih, John R. Kitchin, Drew Higgins, Zachary W. Ulissi, Edward H. Sargent

Bibliographic record

VenueJournal of the American Chemical Society · 2024
Typearticle
Languageen
FieldEnergy
TopicElectrocatalysts for Energy Conversion
Canadian institutionsNational Research Council CanadaBC Innovation CouncilCanadian Light Source (Canada)McMaster UniversityUniversity of Toronto
FundersArgonne National LaboratoryArmy Research OfficeCanada Foundation for InnovationNational Research Council CanadaNatural Sciences and Engineering Research Council of CanadaCanadian Light Source
KeywordsOverpotentialPourbaix diagramChemistryDissolutionCatalysisOxygen evolutionRutheniumHigh-resolution transmission electron microscopyInorganic chemistryChemical engineeringNanotechnologyPhysical chemistryElectrochemistryMaterials scienceTransmission electron microscopyOrganic chemistry

Abstract

fetched live from OpenAlex

The demand for green hydrogen has raised concerns over the availability of iridium used in oxygen evolution reaction catalysts. We identify catalysts with the aid of a machine learning-aided computational pipeline trained on more than 36,000 mixed metal oxides. The pipeline accurately predicts Pourbaix decomposition energy ( G pbx ) from unrelaxed structures with a mean absolute error of 77 meV per atom, enabling us to screen 2070 new metallic oxides with respect to their prospective stability under acidic conditions. The search identifies Ru 0.6 Cr 0.2 Ti 0.2 O 2 as a candidate having the promise of increased durability: experimentally, we find that it provides an overpotential of 267 mV at 100 mA cm –2 and that it operates at this current density for over 200 h and exhibits a rate of overpotential increase of 25 μV h –1 . Surface density functional theory calculations reveal that Ti increases metal–oxygen covalency, a potential route to increased stability, while Cr lowers the energy barrier of the HOO* formation rate-determining step, increasing activity compared to RuO 2 and reducing overpotential by 40 mV at 100 mA cm –2 while maintaining stability. In situ X-ray absorption spectroscopy and ex situ ptychography-scanning transmission X-ray microscopy show the evolution of a metastable structure during the reaction, slowing Ru mass dissolution by 20× and suppressing lattice oxygen participation by >60% compared to RuO 2 .

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 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 score0.004
Threshold uncertainty score0.519

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.001
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)0.0000.000

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 head0.006
GPT teacher head0.232
Teacher spread0.225 · 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.

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

Citations81
Published2024
Admission routes2
Has abstractyes

Explore more

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