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Record W2947177051 · doi:10.1021/jacs.9b03327

Mixed Electron–Proton Conductors Enable Spatial Separation of Bond Activation and Charge Transfer in Electrocatalysis

2019· article· en· W2947177051 on OpenAlexfundno aff
Bing Yan, Ryan P. Bisbey, Alexander Alabugin, Yogesh Surendranath

Bibliographic record

VenueJournal of the American Chemical Society · 2019
Typearticle
Languageen
FieldEnergy
TopicElectrocatalysts for Energy Conversion
Canadian institutionsnot available
FundersDivision of Materials ResearchNational Institute of Environmental Health SciencesCanadian Institute for Advanced ResearchAlfred P. Sloan FoundationHarvard UniversityDivision of ChemistryResearch Corporation for Science AdvancementNational Science Foundation
KeywordsChemistryElectrocatalystChemical physicsElectrolyteElectron transferCatalysisElectrochemistryElectrodeProtonDiffusionPhysical chemistryThermodynamicsOrganic chemistry

Abstract

fetched live from OpenAlex

Electrochemical energy conversion requires electrodes that can simultaneously facilitate substrate bond activation and electron–proton charge transfer. Traditional electrodes co-localize both functions to a single solid|liquid interface even though each process is typically favored in a disparate reaction environment. Herein, we establish a strategy for spatially separating bond activation and charge transfer by exploiting mixed electron–proton conduction (MEPC) in an oxide membrane. Specifically, we interpose a MEPC WO x membrane between a Pt catalyst and aqueous electrolyte and show that this composite electrode is active for the hydrogen oxidation reaction (HOR). Consistent with H 2 activation occurring at the gas|solid interface, the composite electrode displays HOR current densities over 8-fold larger than the diffusion-limited rate of HOR catalysis at a singular Pt|solution interface. The segregation of bond activation and charge separation steps also confers excellent tolerance to poisons and impurities introduced to the electrolyte. Mechanistic studies establish that H 2 activation at the Pt|gas interface is coupled to the electron–proton charge separation at the WO x |solution interface via rapid H-diffusion in the bulk of the WO x . Consequently, the rate of HOR is principally controlled by the rate of H-spillover at the Pt|WO x boundary. Our results establish MEPC membrane electrodes as a platform for spatially separating the critical bond activation and charge transfer steps of 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 integrity0.0000.001
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 head0.007
GPT teacher head0.226
Teacher spread0.219 · 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

Citations27
Published2019
Admission routes1
Has abstractyes

Explore more

Same venueJournal of the American Chemical SocietySame topicElectrocatalysts for Energy ConversionFrench-language works237,207