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Record W4391837607 · doi:10.1002/anie.202319153

Synergistic Lewis and Brønsted Acid Sites Promote OH* Formation and Enhance Formate Selectivity: Towards High‐efficiency Glycerol Valorization

2024· article· en· W4391837607 on OpenAlexaff
Junqing Ma, Xunlu Wang, Junnan Song, Yanfeng Tang, Tongming Sun, Lijia Liu, Jin Wang, Minghui Yang

Bibliographic record

VenueAngewandte Chemie International Edition · 2024
Typearticle
Languageen
FieldEngineering
TopicCatalysis for Biomass Conversion
Canadian institutionsWestern University
FundersProgram of Shanghai Academic Research LeaderScience and Technology Commission of Shanghai MunicipalityNational Natural Science Foundation of ChinaShanghai Anti-Cancer Association
KeywordsGlycerolChemistrySelectivityFormateLewis acids and basesBrønsted–Lowry acid–base theoryCatalysisOrganic chemistryCombinatorial chemistry

Abstract

fetched live from OpenAlex

Abstract As a sustainable valorization route, electrochemical glycerol oxidation reaction (GOR) involves in formation of key OH* and selective adsorption/cleavage of C−C(O) intermediates with multi‐step electron transfer, thus suffering from high potential and poor formate selectivity for most non‐noble‐metal‐based electrocatalysts. So, it remains challenging to understand the structure–property relationship as well as construct synergistic sites to realize high‐activity and high‐selectivity GOR. Herein, we successfully achieve dual‐high performance with low potentials and superior formate selectivity for GOR by forming synergistic Lewis and Brønsted acid sites in Ni‐alloyed Co‐based spinel. The optimized NiCo oxide solid‐acid electrocatalyst exhibits low reaction potential (1.219 V@10 mA/cm 2 ) and high formate selectivity (94.0 %) toward GOR. In situ electrochemical impedance spectroscopy and pH‐dependence measurements show that the Lewis acid centers could accelerate OH* production, while the Brønsted acid centers are proved to facilitate high‐selectivity formation of formate. Theoretical calculations reveal that NiCo alloyed oxide shows appropriate d ‐band center, thus balancing adsorption/desorption of C−O intermediates. This study provides new insights into rationally designing solid‐acid electrocatalysts for biomass electro‐upcycling.

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 score0.002

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 head0.006
GPT teacher head0.216
Teacher spread0.210 · 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

Citations61
Published2024
Admission routes1
Has abstractyes

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Same venueAngewandte Chemie International EditionSame topicCatalysis for Biomass ConversionFrench-language works237,207