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Record W3208881137 · doi:10.33774/chemrxiv-2021-8w57d

Highly efficient water oxidation via a bimolecular reaction mechanism on rutile structured mixed-metal oxyfluorides

2021· preprint· en· W3208881137 on OpenAlexafffund
Zahra Goharibajestani, Xiao Wang, Amandine Guiet, Romain Moury, Jean−Marc Grenèche, Annie Hémon‐Ribaud, Yuxuan Zhang, Daniel Chartrand, V. Maisonneuve, Ali Seifitokaldani, Nikolay Kornienko, Jérôme Lhoste

Bibliographic record

Venuenot available
Typepreprint
Languageen
FieldEnergy
TopicElectrocatalysts for Energy Conversion
Canadian institutionsUniversité de MontréalMcGill University
FundersNatural Sciences and Engineering Research Council of CanadaFonds de recherche du Québec – Nature et technologiesCentre National de la Recherche ScientifiqueCompute Canada
KeywordsOverpotentialTafel equationCatalysisRutileElectrocatalystOxygen evolutionChemical engineeringElectrochemistryMaterials scienceInorganic chemistryMetalChemistryElectrodePhysical chemistryMetallurgy

Abstract

fetched live from OpenAlex

Mixed-metal oxides are generally considered to be the highest-performance catalysts for alkaline water oxidation. Despite significant efforts dedicated to understanding and accelerating their efficiency, most works have been limited investigations of Ni, Co, and Fe oxides, thus overlooking beneficial effects of hetero-anion incorporation. To this end, we report on the development of Co0.5Fe0.5O0.5F1.5 oxyfluoride materials featuring a rutile crystal structure and porous morphology via a scalable and green synthetic route. The catalyst surface, enhanced through electron withdrawing effects imparted by the fluoride ions, give rise to highly effective catalytic sites for electrochemical water oxidation. In particular, their performance across metrics of Tafel slope (27 mV/dec), mass activity (846 A/g at 1.53 V vs. RHE), turnover frequency (21/s at 1.53 V vs. RHE), overpotential (220 mV for 10 mA/cm2), and stability (27 days of continuous operation) largely surpasses most known Co-based catalysts. Mechanistic studies suggest that this performance is driven by a bimolecular, oxygen coupling reaction mechanism through proximal active sites on the catalyst surface, thus enabling a new avenue for achieving accelerated oxygenic electrocatalysis.

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 score0.003

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 science0.0000.000
Research integrity0.0000.000
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 head0.006
GPT teacher head0.203
Teacher spread0.197 · 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

Citations0
Published2021
Admission routes2
Has abstractyes

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