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Record W4309646813 · doi:10.1021/acscatal.2c03675

Machine-Learning-Driven High-Entropy Alloy Catalyst Discovery to Circumvent the Scaling Relation for CO<sub>2</sub> Reduction Reaction

2022· article· en· W4309646813 on OpenAlex
Zhiwen Chen, Zachary Gariepy, Lixin Chen, Xue Yao, Abu Anand, Szu-Jia Liu, Conrard Giresse Tetsassi Feugmo, Isaac Tamblyn, Chandra Veer Singh

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.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.
fundA Canadian funder is recorded on the work.

Bibliographic record

VenueACS Catalysis · 2022
Typearticle
Languageen
FieldEnergy
TopicElectrocatalysts for Energy Conversion
Canadian institutionsUniversity of OttawaVector InstituteNational Research Council CanadaUniversity of Toronto
FundersNatural Sciences and Engineering Research Council of CanadaUniversity of Toronto
KeywordsCatalysisScalingAdsorptionDensity functional theoryChemistryRedoxEntropy (arrow of time)ElectrochemistryThermodynamicsIsothermal processChemical physicsComputational chemistryMaterials sciencePhysical chemistryInorganic chemistryMathematicsPhysicsOrganic chemistry

Abstract

fetched live from OpenAlex

To achieve an equitable energy transition toward net-zero 2050 goals, the electrochemical reduction of CO2 (CO2RR) to chemical feedstocks through utilizing both CO2 and renewable energy is particularly attractive. However, the catalytic activity of CO2RR is limited by the scaling relation of the adsorption energies of intermediates. Circumventing the scaling relation is a potential strategy to achieve a breakthrough in catalytic activity. Herein, based on density functional theory (DFT) calculations, we designed a high-entropy alloy (HEA) system of FeCoNiCuMo with high catalytic activity for CO2RR. Machine learning models were developed by considering 1280 adsorption sites to predict the adsorption energies of COOH*, CO*, and CHO*. The scaling relation between the adsorption energies of COOH*, CO*, and CHO* is circumvented by the rotation of COOH* and CHO* on the designed HEA surface, resulting in the outstanding catalytic activity of CO2RR with the limiting potential of 0.29–0.51 V. This work not only accelerates the development of HEA catalysts but also provides an effective strategy to circumvent the scaling relation.

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)0.001
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow), Science and technology studies
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 score0.184
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.001
Science and technology studies0.0020.000
Scholarly communication0.0000.001
Open science0.0010.000
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 head0.008
GPT teacher head0.214
Teacher spread0.207 · 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