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Record W3105323469 · doi:10.1021/acs.chemmater.0c03260

Modeling Exsolution of Pt from ATiO<sub>3</sub> Perovskites (A = Ca/Sr/Ba) Using First-Principles Methods

2020· article· en· W3105323469 on OpenAlex

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

fundA Canadian funder is recorded on the work.
no affNo Canadian affiliation: this work is invisible to an affiliation-only frame.
No Canadian affiliation. An affiliation-only frame, the usual design, would never have seen this work. It is one of the works that make the case for inverting the frame.

Bibliographic record

VenueChemistry of Materials · 2020
Typearticle
Languageen
FieldMaterials Science
TopicElectronic and Structural Properties of Oxides
Canadian institutionsnot available
FundersAir Force Office of Scientific ResearchCanadian Institute for Advanced Research
KeywordsPerovskite (structure)DopantDensity functional theoryMaterials scienceMolecular dynamicsAb initioChemical physicsDopingAb initio quantum chemistry methodsDiffusionNanotechnologyChemistryComputational chemistryCrystallographyThermodynamicsMoleculePhysicsOptoelectronics

Abstract

fetched live from OpenAlex

Exsolution of transition metals from host perovskites has emerged as a unique synthesis method for designing catalysts for energy applications. Here, using accurate first-principles density functional theory, coupled with an ab initio steered molecular dynamics and umbrella sampling framework, we rationalize both the energetics as well as the dynamics of the exsolution process of a quintessential system: Pt-doped ATiO3 (A = Ca/Sr/Ba) perovskites and identify the major driving forces for Pt exsolution. From the developed ab initio thermodynamic framework, we find that Pt exsolution from ATiO3 (A = Ca/Sr/Ba) perovskites has a distinct host-perovskite facet dependence and likely proceeds through sub-surface vacancy formation followed by diffusion of the doped Pt to the surface of the host perovskite. The molecular dynamics simulations reveal that the exsolution process has a clear temperature and host-perovskite dependence, establishing that only specific dopant-host perovskite combinations at favorable thermophysical conditions result in the catalyst with the novel properties. This opens new paths for the predictive synthesis of intelligent catalysts.

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.

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)0.000
metaresearch head score (Gemma)0.001
Version: codex-gemma-dda1882f352aValidation 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 score0.021
Threshold uncertainty score0.804

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
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 head0.063
GPT teacher head0.280
Teacher spread0.217 · 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