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Record W3196457189 · doi:10.1038/s41467-021-25573-9

Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites

2021· article· en· W3196457189 on OpenAlex
Le Li, Adnan Ozden, Shuyi Guo, F. Pelayo Garcı́a de Arquer, Chuanhao Wang, Mingzhe Zhang, Jin Zhang, Haoyang Jiang, Wei Wang, Hao Dong, David Sinton, Edward H. Sargent, Miao Zhong

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.

Bibliographic record

VenueNature Communications · 2021
Typearticle
Languageen
FieldEnergy
TopicCO2 Reduction Techniques and Catalysts
Canadian institutionsUniversity of Toronto
FundersNanjing UniversityGovernment of Jiangsu ProvinceNatural Science Foundation of Jiangsu ProvinceNational Natural Science Foundation of China
KeywordsFormateOverpotentialFaraday efficiencyRedoxElectrocatalystElectrochemistryFormic acidActive siteChemistryInorganic chemistryMaterials scienceChemical engineeringElectrodeCatalysisPhysical chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Abstract Electrochemical reduction of CO 2 (CO 2 R) to formic acid upgrades waste CO 2 ; however, up to now, chemical and structural changes to the electrocatalyst have often led to the deterioration of performance over time. Here, we find that alloying p-block elements with differing electronegativities modulates the redox potential of active sites and stabilizes them throughout extended CO 2 R operation. Active Sn-Bi/SnO 2 surfaces formed in situ on homogeneously alloyed Bi 0.1 Sn crystals stabilize the CO 2 R-to-formate pathway over 2400 h (100 days) of continuous operation at a current density of 100 mA cm −2 . This performance is accompanied by a Faradaic efficiency of 95% and an overpotential of ~ −0.65 V. Operating experimental studies as well as computational investigations show that the stabilized active sites offer near-optimal binding energy to the key formate intermediate *OCHO. Using a cation-exchange membrane electrode assembly device, we demonstrate the stable production of concentrated HCOO – solution (3.4 molar, 15 wt%) over 100 h.

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.

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 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 score0.083
Threshold uncertainty score0.652

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.001
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.001
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 head0.016
GPT teacher head0.299
Teacher spread0.283 · 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