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Record W4400201634 · doi:10.26434/chemrxiv-2024-bfv3d

A Foundational Model for Reaction Networks on Metal Surfaces

2024· preprint· en· W4400201634 on OpenAlexaff
Santiago Morandi, Oliver Loveday, Tim Renningholtz, Sergio Pablo‐García, Rodrigo A. Vargas–Hernández, Ranga Rohit Seemakurthi, Pol Sanz Berman, Rodrigo García‐Muelas, Alán Aspuru‐Guzik, Núria López

Bibliographic record

VenueChemRxiv · 2024
Typepreprint
Languageen
FieldMaterials Science
TopicMachine Learning in Materials Science
Canadian institutionsCanadian Institute for Advanced ResearchVector InstituteMcMaster UniversityUniversity of Toronto
FundersHorizon 2020Office of ScienceEuropean CommissionNCCR CatalysisErasmus+University of MinnesotaU.S. Department of EnergySchweizerischer Nationalfonds zur Förderung der Wissenschaftlichen ForschungGeneralitat de CatalunyaNational Science Foundation
KeywordsCatalysisChemistryComputer scienceBiochemical engineeringOrganic chemistryEngineering

Abstract

fetched live from OpenAlex

Process optimization in heterogeneous catalysis relies on the control of competing reactions. The reaction mechanisms based on chemical knowledge can be evaluated via density functional theory unveiling experimental catalytic trends. However, this approach finds its limits when applied to complex reaction networks or large molecules, disregarding alternative paths and rare events. Here we present CARE, a foundational model for catalysis on metal surfaces with a rule-based reaction network generator for CxHyOz species built with GAME-Net-UQ, a graph neural network with uncertainty quantification targeting thermodynamic and kinetic parameters, coupled to microkinetic modeling. CARE reproduces experimental activity trends in methanol decomposition, selectivity to C3 products in electrochemical reduction processes, and models the Fischer-Tropsch synthesis to C6 products, including 370k reactions, breaking the current limits of network exploration. This comprehensive model opens the path towards the exploration of thermal and electrocatalytic surface processes previously not amenable to atomistic simulations.

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)0.002
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: Simulation or modeling · Consensus signal: Simulation or modeling
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.294
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0020.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0010.000
Open science0.0010.001
Research integrity0.0000.001
Insufficient payload (model declined to judge)0.0000.000

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 head0.040
GPT teacher head0.313
Teacher spread0.273 · 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 designSimulation or modeling
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

Citations6
Published2024
Admission routes1
Has abstractyes

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