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Record W4381245510 · doi:10.1021/acs.jpcc.3c02705

Machine Learning Based Electronic Structure Predictors in Single-Atom Alloys: A Model Study of CO Kink-Site Adsorption across Transition Metal Substrates

2023· article· en· W4381245510 on OpenAlexafffund
Javad Shirani, Hanh D. M. Pham, Shuaishuai Yuan, Alain Tchagang, Julio J. Valdés, Kirk H. Bevan

Bibliographic record

VenueThe Journal of Physical Chemistry C · 2023
Typearticle
Languageen
FieldEnergy
TopicCO2 Reduction Techniques and Catalysts
Canadian institutionsNational Research Council CanadaMcGill University
FundersNational Research Council CanadaFaculty of Engineering, McGill University
KeywordsAdsorptionElectronic structureAtom (system on chip)Substrate (aquarium)Electronic band structureSpace (punctuation)Chemical physicsTransition metalMaterials scienceBand gapChemistryComputational chemistryComputer scienceCondensed matter physicsPhysical chemistryPhysicsOptoelectronics

Abstract

fetched live from OpenAlex

This work reports on a comprehensive analysis of the predictive capacity and underlying physicochemical trends provided by d -band based electronic structure features as applied to single-atom alloys (SAAs). Taking CO adsorption energies at kink sites as a model framework, SAA adsorption trends are examined across a range of substrates with vastly differing intrinsic CO adsorption trends. Through this approach, it is demonstrated that SAA adsorption properties can be highly transferable, often displaying atom-like behavior independent of the host substrate, particularly in groups 6 through 12 of the periodic table. The predictability of such SAA behavior is found, however, to be highly qualitative for single d -band based electronic structure features. Nevertheless, it is shown that predictive capacity can be greatly improved through the creation of a feature space comprised of as few as 8 electronic structure features. Intriguingly, following the framework of Hammer and Nørskov, the machine learning accuracy of d -band based electronic structure features is shown to be sensitive to the atomic configuration diversity present in the training ensemble with model accuracy systematically improving through restrictions in the configurational space. More directly, it is shown that elements to the far left of the transition metal block such as Zr and Hf may exhibit CO binding properties comparable to Cu in the CO 2 reduction reaction. However, impurities from groups 6–10 are demonstrated to overbind in a highly transferable manner in line with established pure substrate trends and are likely to act as unwanted posing species concerning CO and the overall CO 2 reduction reaction. The results of this work broadly lay out the predictive capabilities of d -band features as applied to SAAs, as well as their propensity for exhibiting transferable binding properties among d -band substrates.

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)0.001
Version: metacan-v3-hybrid-931329e0061cValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Simulation or modeling · Consensus signal: Simulation or modeling
GenreCandidate signal: Methods · Consensus signal: none
Teacher disagreement score0.004
Threshold uncertainty score0.008

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.001
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0010.000
Open science0.0010.000
Research integrity0.0010.000
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 head0.011
GPT teacher head0.259
Teacher spread0.248 · 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 designSimulation or modeling
Domainnot available
GenreMethods

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

Citations6
Published2023
Admission routes2
Has abstractyes

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