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Record W4405802211 · doi:10.1002/anie.202423915

Simultaneous High Current Density and Selective Electrocatalytic CO<sub>2</sub>‐to‐CH<sub>4</sub> through Intermediate Balancing

2024· article· en· W4405802211 on OpenAlexaff
Shuqi Hu, Yumo Chen, Zhiyuan Zhang, Heming Liu, Xin Kang, Jiarong Liu, Shanlin Li, Yuting Luo, Bilu Liu

Bibliographic record

VenueAngewandte Chemie International Edition · 2024
Typearticle
Languageen
FieldEnergy
TopicCO2 Reduction Techniques and Catalysts
Canadian institutionsUniversity of Toronto
FundersTsinghua Shenzhen International Graduate SchoolDivision of Materials ResearchBasic and Applied Basic Research Foundation of Guangdong ProvinceNational Science Fund for Distinguished Young ScholarsNational Natural Science Foundation of ChinaShenzhen Fundamental Research ProgramDepartment of Education of Guangdong Province
KeywordsFaraday efficiencySelectivityElectrosynthesisCatalysisCoupling (piping)Current densityElectrochemistryWork (physics)ChemistryMaterials scienceChemical engineeringElectrodePhysical chemistryOrganic chemistryThermodynamics

Abstract

fetched live from OpenAlex

Abstract The electrochemical reduction of CO 2 to CH 4 is promising for carbon neutrality and renewable energy storage but confronts low CH 4 selectivity, especially at high current densities. The key challenge lies in promoting *CO intermediate and *H coupling while minimizing side reactions including C−C coupling and H−H coupling, which is particularly difficult at high current density due to abundant intermediates. Here we report a cooperative strategy to address this challenge using Cu‐based catalysts comprising Cu−N coordination polymer and CuO component that can simultaneously manage the key intermediates *CO and *H. A fast CO 2 ‐to‐CH 4 conversion rate of 3.14 mmol cm −2 h −1 is achieved at 1,300 mA cm −2 with a Faradaic efficiency of 51.7 %. In situ spectroscopy and theoretical calculations show that the increased Cu−Cu distance in the Cu−N coordination polymer component favors multistep *CO hydrogenation over the dimerization, and the CuO component ensures an adequate supply of *H, together contributing to the selective CO 2 ‐to‐CH 4 conversion at high current densities. This work develops a cooperative strategy for the electrosynthesis of CH 4 with simultaneous high current density and high selectivity by rational catalyst design, paving the way for its applications.

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 score0.006

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0010.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.001
Open science0.0010.001
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 head0.008
GPT teacher head0.257
Teacher spread0.250 · 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

Citations22
Published2024
Admission routes1
Has abstractyes

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