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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 OpenAlex

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

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.

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 score0.165
Threshold uncertainty score0.697

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 communication0.0000.001
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 head0.006
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