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Record W4288695396 · doi:10.1021/jacs.2c01044

Mechanistic Insights into OC–COH Coupling in CO<sub>2</sub> Electroreduction on Fragmented Copper

2022· article· en· W4288695396 on OpenAlexaff
Kaili Yao, Jun Li, Haibin Wang, Ruihu Lu, Xiaotao Yang, Mingchuan Luo, Ning Wang, Ziyun Wang, Changxu Liu, Tan Jing, Songhua Chen, Emiliano Cortés, Stefan A. Maier, Sheng Zhang, Tieliang Li, Yifu Yu, Yongchang Liu, Xinchen Kang, Hongyan Liang

Bibliographic record

VenueJournal of the American Chemical Society · 2022
Typearticle
Languageen
FieldEnergy
TopicCO2 Reduction Techniques and Catalysts
Canadian institutionsUniversity of Toronto
FundersH2020 European Research CouncilEngineering and Physical Sciences Research CouncilSolar Technologies go HybridQinghai Nationalities UniversityDeutsche ForschungsgemeinschaftDepartment of Education, Fujian ProvinceCenter for NanoScience, Ludwig-Maximilians-Universität MünchenNational Natural Science Foundation of China
KeywordsChemistryCopperCoupling (piping)ElectrochemistryComputational chemistryInorganic chemistryElectrodePhysical chemistryMetallurgyOrganic chemistry

Abstract

fetched live from OpenAlex

The carbon–carbon (C–C) bond formation is essential for the electroconversion of CO 2 into high-energy-density C 2+ products, and the precise coupling pathways remain controversial. Although recent computational investigations have proposed that the OC–COH coupling pathway is more favorable in specific reaction conditions than the well-known CO dimerization pathway, the experimental evidence is still lacking, partly due to the separated catalyst design and mechanistic/spectroscopic exploration. Here, we employ density functional theory calculations to show that on low-coordinated copper sites, the *CO bindings are strengthened, and the adsorbed *CO coupling with their hydrogenation species, *COH, receives precedence over CO dimerization. Experimentally, we construct a fragmented Cu catalyst with abundant low-coordinated sites, exhibiting a 77.8% Faradaic efficiency for C 2+ products at 300 mA cm –2 . With a suite of in situ spectroscopic studies, we capture an *OCCOH intermediate on the fragmented Cu surfaces, providing direct evidence to support the OC–COH coupling pathway. The mechanistic insights of this research elucidate how to design materials in favor of OC–COH coupling toward efficient C 2+ production from CO 2 reduction.

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)0.000
Version: metacan-v3-hybrid-931329e0061cValidation 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 score0.002
Threshold uncertainty score0.005

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.001
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0020.000

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 head0.007
GPT teacher head0.242
Teacher spread0.235 · 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 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

Citations217
Published2022
Admission routes1
Has abstractyes

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