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Record W4389923081 · doi:10.1021/acscatal.3c04310

Spontaneous Demetallation of Mn<sup>(II)</sup>N<sub><i>x</i></sub> Catalytic Sites in Proton Exchange Membrane Fuel Cell Conditions

2023· article· en· W4389923081 on OpenAlexafffund
Vassili P. Glibin, Jean‐Pol Dodelet, Gaixia Zhang

Bibliographic record

VenueACS Catalysis · 2023
Typearticle
Languageen
FieldEnergy
TopicElectrocatalysts for Energy Conversion
Canadian institutionsÉcole de Technologie SupérieureInstitut National de la Recherche ScientifiqueWestern University
FundersNatural Sciences and Engineering Research Council of CanadaÉcole de technologie supérieureInstitut national de la recherche scientifique
KeywordsCatalysisChemistryManganeseInorganic chemistryProton exchange membrane fuel cellElectrochemistryLeaching (pedology)Transition metalGibbs free energyOxidation stateDivalentAdsorptionChemical stabilityPhysical chemistryOrganic chemistryElectrode

Abstract

fetched live from OpenAlex

The present work is about a thermodynamic assessment of the stability behavior of several Mn (II) N x - and Mn (III) N x /C active sites in Mn/N/C catalysts at 298 and 353 K (80 °C) in the acidic environment of proton exchange membrane (PEM) fuel cells. The calculated Gibbs free energies for the manganese ion leaching reaction indicate that all Mn (II) N x active sites considered in this work are unstable in these conditions. However, the opposite is observed when a three-valent state is adopted for the Mn ion. The transition of manganese from the divalent to the trivalent state is accompanied by the addition of an axial ligand (particularly, by an O 2 molecule). The adsorption of an O 2 molecule to the metal ion of the sites to obtain O 2 ···Mn (III) N 4 /C, O 2 ···Mn (III) N (2+2) /C, or O 2 ···Mn (III) N (4+2) /C leads to highly resisting sites to acid leaching at 298 and 353 K. The thermodynamic stability toward acid leaching is also analyzed for the de-oxygenated Mn (III) N 4 /C, Mn (III) N (2+2) /C, and Mn (III) N (4+2) /C sites. Such sites are also rather stable toward demetallation. In addition, the importance of other aspects (Fenton reaction, electrochemical functionalization/corrosion) affecting the stability of Mn/N/C and Fe/N/C catalysts is also discussed. From this discussion, it is concluded that, contrary to demetallation and also to electro-functionalization/oxidation, Fenton reaction is not an important cause of instability either for Mn/N/C or for Fe/N/C cathode catalysts in fuel cells.

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 categoriesMeta-epidemiology (narrow)
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 score0.035
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0010.004
Science and technology studies0.0000.000
Scholarly communication0.0000.001
Open science0.0010.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0000.001

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 head0.010
GPT teacher head0.216
Teacher spread0.206 · 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.

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

Citations8
Published2023
Admission routes2
Has abstractyes

Explore more

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