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Record W4225316143 · doi:10.1002/chem.202200340

Electrocatalysts Derived from Copper Complexes Transform CO into C <sub>2+</sub> Products Effectively in a Flow Cell

2022· article· en· W4225316143 on OpenAlexafffund
Shaoxuan Ren, Zishuai Zhang, Eric W. Lees, Arthur G. Fink, Luke Melo, Camden Hunt, David Dvořák, Wen Yu Wu, Edward R. Grant, Curtis P. Berlinguette

Bibliographic record

VenueChemistry - A European Journal · 2022
Typearticle
Languageen
FieldEnergy
TopicCO2 Reduction Techniques and Catalysts
Canadian institutionsCanadian Institute for Advanced ResearchUniversity of British Columbia
FundersCanada First Research Excellence FundCanadian Network for Research and Innovation in Machining Technology, Natural Sciences and Engineering Research Council of CanadaCanada Research ChairsCanadian Institute for Advanced Research
KeywordsCatalysisCopperChemistryElectrolysisBulk electrolysisElectrocatalystInorganic chemistryFaraday efficiencyElectrolyteElectrochemistryMetalHydroxideChemical engineeringElectrodeOrganic chemistryPhysical chemistry

Abstract

fetched live from OpenAlex

Abstract Electrochemical reactors that electrolytically convert CO 2 into higher‐value chemicals and fuels often pass a concentrated hydroxide electrolyte across the cathode. This strongly alkaline medium converts the majority of CO 2 into unreactive HCO 3 − and CO 3 2− byproducts rather than into CO 2 reduction reaction (CO2RR) products. The electrolysis of CO (instead of CO 2 ) does not suffer from this undesirable reaction chemistry because CO does not react with OH − . Moreover, CO can be more readily reduced into products containing two or more carbon atoms (i. e., C 2+ products) compared to CO 2 . We demonstrate here that an electrocatalyst layer derived from copper phthalocyanine ( CuPc ) mediates this conversion effectively in a flow cell. This catalyst achieved a 25 % higher selectivity for acetate formation at 200 mA/cm 2 than a known state‐of‐art oxide‐derived Cu catalyst tested in the same flow cell. A gas diffusion electrode coated with CuPc electrolyzed CO into C 2+ products at high rates of product formation (i. e., current densities ≥200 mA/cm 2 ), and at high faradaic efficiencies for C 2+ production ( FE C2+ ; >70 % at 200 mA/cm 2 ). While operando Raman spectroscopy did not reveal evidence of structural changes to the copper molecular complex, X‐ray photoelectron spectroscopy suggests that the catalyst undergoes conversion to a metallic copper species during catalysis. Notwithstanding, the ligand environment about the metal still impacts catalysis, which we demonstrated through the study of a homologous CuPc bearing ethoxy substituents. These findings reveal new strategies for using metal complexes for the formation of carbon‐neutral chemicals and fuels at industrially relevant conditions.

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 score0.001
Threshold uncertainty score0.003

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 studies0.0000.000
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 head0.008
GPT teacher head0.207
Teacher spread0.200 · 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

Citations17
Published2022
Admission routes2
Has abstractyes

Explore more

Same venueChemistry - A European JournalSame topicCO2 Reduction Techniques and CatalystsFrench-language works237,207