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Record W4376255872 · doi:10.26434/chemrxiv-2023-g2rj1

In-situ Studies of Copper-based CO2 Reduction Electrocatalystsby Scanning Transmission Soft X-ray Microscopy

2023· preprint· en· W4376255872 on OpenAlexafffund
Chunyang Zhang, Haytham Eraky, Shunquan Tan, Adam P. Hitchcock, Drew Higgins

Bibliographic record

VenueChemRxiv · 2023
Typepreprint
Languageen
FieldBiochemistry, Genetics and Molecular Biology
TopicAdvanced Electron Microscopy Techniques and Applications
Canadian institutionsMcMaster University
FundersNatural Sciences and Engineering Research Council of CanadaCanadian Institutes of Health ResearchUniversity of Saskatchewan
KeywordsElectrodeElectrochemistryMaterials scienceCatalysisCopperChemical engineeringRedoxMetalOxideNanotechnologyElectrocatalystAnalytical Chemistry (journal)ChemistryMetallurgyPhysical chemistry

Abstract

fetched live from OpenAlex

A micro-fluidic enabled electrochemical device has been developed to investigate electrochemically active materials under reaction conditions using in-situ scanning transmission soft X-ray microscopy (STXM). In-situ STXM measurements at the Cu 2p edge were conducted on electro-deposited Cu catalysts under electrochemical CO2 reduction (CO2R) conditions. The study provides detailed, quantitative results about the changes in the morphology and chemical structure (oxidation state) of the catalyst particles as a function of applied electrode potentials. The initially electrochemically deposited Cu particles contain both Cu(0) and Cu(I). As an increasingly cathodic potential is applied, the Cu(I) species gradually converted to Cu(0) over the potential range of +0.4 to 0 V versus the reversible hydrogen electrode (VRHE). During this process, Cu(I) particles of various sizes are converted to metallic Cu at different reaction rates and at slightly different electrode potentials, indicating a degree of heterogeneity in the electrochemical response of discrete particles. At CO2R relevant potentials, only metallic Cu is observed, and the morphology of the particles is fairly stable within the spatial resolution limits of STXM (~ 40 nm). We also prepared a working electrode with relatively thick Cu-based electro-deposits. The spatially resolved chemical analysis by STXM identified that Cu-oxide species can persist under CO2R conditions, but only when the catalyst particles are electronically isolated from the working electrode and therefore are catalytically irrelevant. Thus, in-situ STXM is presented as a technique to gain advanced morphological and spatially-resolved chemical structure insight into electrochemically active materials, which was used to provide improved understanding regarding Cu electrodes under CO2 reaction 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 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)0.000
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: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.056
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

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)0.0000.000

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 head0.022
GPT teacher head0.359
Teacher spread0.337 · 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 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

Citations2
Published2023
Admission routes2
Has abstractyes

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