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Record W4415525951 · doi:10.1021/jacs.5c12052

Direct Electrosynthesis of C <sub>3+</sub> Hydrocarbons from CO <sub>2</sub> via Size-Controlled Nickel Nanoislands on a Carbon Support

2025· article· en· W4415525951 on OpenAlexafffund
Maral Vafaie, Roham Dorakhan, Amin Morteza Najarian, Zahra Teimouri-Jervekani, Alexandre Pofelski, Nasim Barati, Ching-Hsuan Chou, Ya‐Ching Chang, Sung‐Fu Hung, Qian Sun, Zahra Azimi Dijvejin, Robert Ngunjiri, Yuke Li, Ali Shayesteh Zeraati, Kholoud E. Salem, Rui Kai Miao, Sjoerd Hoogland, Drew Higgins, Edward H. Sargent, David Sinton

Bibliographic record

VenueJournal of the American Chemical Society · 2025
Typearticle
Languageen
FieldEnergy
TopicCO2 Reduction Techniques and Catalysts
Canadian institutionsDiscovery CentreMcMaster UniversityUniversity of Toronto
FundersNatural Sciences and Engineering Research Council of CanadaCanada Research Chairs
KeywordsHydrocarbonElectrosynthesisNickelAdsorptionElectrochemistryNanoparticleCarbon fibersCyclic voltammetry

Abstract

fetched live from OpenAlex

Direct synthesis of C 3+ hydrocarbons via the electrochemical CO 2 reduction reaction is highly desirable for producing sustainable chemicals. However, this approach remains challenging due to the limited ability of current electrocatalysts to adsorb and couple key reaction intermediates effectively, with promising systems, such as Ni oxyhydroxide-derived catalysts, still exhibiting partial current densities toward C 3+ hydrocarbons <0.9 mA cm –2 . Motivated by the limited activity and control over the active site environment of these systems, we hypothesize that reducing the size of metallic Ni modifies its electronic states and introduces interfacial metal–support sites that promote more balanced *CO adsorption, critical for facilitating C–C coupling beyond C 2 intermediates. Here, we report a plasma-assisted deposition method to synthesize size-controlled metallic Ni nanoislands on a carbon support. Characterization revealed that reducing the nanoisland size (<12 nm) forms undercoordinated, electron-deficient, and strained surfaces with a downshifted d-band center─features associated with weakened *CO binding, favoring intermediate coupling and C 3+ hydrocarbon formation. Nanoislands as small as ∼3.5 nm delivered a 120-fold increase in C 3+ hydrocarbon specific activity relative to large particles (bulk-like Ni). CO stripping voltammetry shows weaker *CO adsorption on isolated nanoislands. While C 3+ partial current densities remain low (∼0.1 mA cm –2 ), these findings identify nanoparticle size and metal–support interactions as key design parameters for advancing CO 2 conversion to long-chain hydrocarbons, offering a foundation for further improvement, as demonstrated by a >20-fold enhancement in the Ni-mass-based activity versus state-of-the-art catalysts.

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 score0.004

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 head0.004
GPT teacher head0.221
Teacher spread0.217 · 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

Citations6
Published2025
Admission routes2
Has abstractyes

Explore more

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