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Record W4388735123 · doi:10.26434/chemrxiv-2023-3l19q

The Cationic Enhancement Effect on the Two-Electron Oxygen Reduction Reaction in Acidic Conditions at Carbon-Based Cathodes

2023· preprint· en· W4388735123 on OpenAlexaff
Jessica Hübner, Lanna E.B. Lucchetti, Hong Nhan Nong-Reier, Benjamin Paul, Matthias Kroschel, Jiaqi Kang, Detre Teschner, Silke Behrens, Felix Studt, Axel Knop‐Gericke, Samira Siahrostami, Peter Strasser

Bibliographic record

VenueChemRxiv · 2023
Typepreprint
Languageen
FieldEnergy
TopicElectrocatalysts for Energy Conversion
Canadian institutionsSimon Fraser University
FundersBundesministerium für Bildung und ForschungFundação de Amparo à Pesquisa do Estado de São PauloDeutsche Forschungsgemeinschaft
KeywordsChemistryCatalysisPoint of zero chargeElectrochemistryElectrolyteHydrogen peroxideInorganic chemistryAnodeCarbon fibersOxygen evolutionOxygenReversible hydrogen electrodeCationic polymerizationElectrodeMaterials scienceAqueous solutionPhysical chemistryWorking electrodeOrganic chemistry

Abstract

fetched live from OpenAlex

Hydrogen peroxide (H2O2) is a green oxidant, widely used in industry. To turn its synthesis green, research focused on the development of efficient catalysts for the two-electron oxygen reduction reaction (2e-ORR) to produce H2O2 from water and molecular oxygen. Despite recent progress, electrolyte effects of the electrochemical H2O2 production have remained little understood. We report a significant effect of alkali metal cations (AMCs) on the electrocatalytic H2O2 production on carbon catalysts in acidic environments. The presence of AMCs at the electrified carbon interface shift the half wave potential of the 2e-ORR from -0.48 V to -0.22 VRHE. This cationic induced enhancement effect exhibits a uniquely sensitive on/off switching behaviour depending on the voltammetric protocol. Voltammetric and direct in situ X-ray photoemission spectroscopic evidence is presented that supports a controlling role of the potential of zero charge (PZC) of the catalytic enhancement. Depending whether the electrode potential is kept cathodic or even just briefly reaches values anodic of the PZC, AMCs accumulate at the electrified interface and enhance the 2e-ORR or get repelled away from it, respectively. Density functional theory calculations associate the enhancement by the stabilization of the *OOH key intermediate. Based on this finding, we developed a refined reaction mechanism for the H2O2 production in presence of AMCs.

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 score0.005

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 communication0.0000.000
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 head0.016
GPT teacher head0.266
Teacher spread0.250 · 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
Published2023
Admission routes1
Has abstractyes

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