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Record W4309665479 · doi:10.1002/anie.202216062

Boosting Benzene Oxidation with a Spin‐State‐Controlled Nuclearity Effect on Iron Sub‐Nanocatalysts

2022· article· en· W4309665479 on OpenAlexaff
Fanle Bu, Chaoqiu Chen, Yu Yu, Wentao Hao, Shichao Zhao, Yongfeng Hu, Yong Qin

Bibliographic record

VenueAngewandte Chemie International Edition · 2022
Typearticle
Languageen
FieldMaterials Science
TopicCatalytic Processes in Materials Science
Canadian institutionsUniversity of Saskatchewan
FundersNational Science Fund for Distinguished Young ScholarsNatural Science Foundation of Shanxi ProvinceNational Natural Science Foundation of China
KeywordsNanomaterial-based catalystCatalysisTrimerNanorodBenzeneTetramerChemistrySpin statesOxidation stateDimerMaterials scienceCrystallographyNanotechnologyPhotochemistryInorganic chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Abstract A fundamental understanding of the nature of nuclearity effects is important for the rational design of superior sub‐nanocatalysts with low nuclearity, but remains a long‐standing challenge. Using atomic layer deposition, we precisely synthesized Fe sub‐nanocatalysts with tunable nuclearity (Fe 1 –Fe 4 ) anchored on N,O‐co‐doped carbon nanorods (NOC). The electronic properties and spin configuration of the Fe sub‐nanocatalysts were nuclearity dependent and dominated the H 2 O 2 activation modes and adsorption strength of active O species on Fe sites toward C−H oxidation. The Fe 1 ‐NOC single atom catalyst exhibits state‐of‐the‐art activity for benzene oxidation to phenol, which is ascribed to its unique coordination environment (Fe 1 N 2 O 3 ) and medium spin state ( t 2g 4 e g 1 ); turnover frequencies of 407 h −1 at 25 °C and 1869 h −1 at 60 °C were obtained, which is 3.4, 5.7, and 13.6 times higher than those of Fe dimer, trimer, and tetramer catalysts, respectively.

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)0.001
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesInsufficient payload (model declined to judge)
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 score0.006
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
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 science0.0010.000
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 head0.007
GPT teacher head0.244
Teacher spread0.237 · 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

Citations34
Published2022
Admission routes1
Has abstractyes

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