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Record W4366580344 · doi:10.1021/acscatal.3c00513

Identifying the Activity Origin of a Single-Atom Au<sub>1</sub>/Nb<sub>2</sub>O<sub>5</sub> Catalyst for Hydrodeoxygenation of Methylcatechol: A Stable Substitutional Au<sup>+</sup> Site

2023· article· en· W4366580344 on OpenAlexaff
Jie Xia, Xiaohui Liu, Roman Chernikov, Mohsen Shakouri, Yongfeng Hu, Yong Guo, Jianjian Wang, Kepeng Song, P. Hu, Yanqin Wang, Haifeng Wang

Bibliographic record

VenueACS Catalysis · 2023
Typearticle
Languageen
FieldEngineering
TopicCatalysis and Hydrodesulfurization Studies
Canadian institutionsCanadian Light Source (Canada)
FundersHigher Education Discipline Innovation ProjectScience and Technology Commission of Shanghai MunicipalityMinistry of Science and Technology of the People's Republic of ChinaNational Natural Science Foundation of China
KeywordsHydrodeoxygenationCatalysisHeterolysisDensity functional theoryChemistryCrystallographyAtom (system on chip)Dissociation (chemistry)Computational chemistryPhysical chemistryOrganic chemistrySelectivity

Abstract

fetched live from OpenAlex

Developing effective and stable single-atom catalysts (SACs) is a significant but challenging task, which requires the identification of single-atom metal sites and their configurations. Herein, we report a single-atom Au 1 /Nb 2 O 5 catalyst for the hydrodeoxygenation of methylcatechol, a lignin model compound, which maintains stability in five consecutive conversions. Combined with the density functional theory (DFT) calculations, the Au + located at the Nb lattice site with two concomitant oxygen vacancies (Au@Nb v –2O v ) is identified as the thermodynamically favorable Au single-atom species and dominates the activity for molecular H 2 dissociation via a heterolytic mechanism. Moreover, the presence of oxygen vacancies in Au@Nb v –2O v facilitates the adsorption of methylcatechol, resulting in efficient cleavage of C–O bonds. Consequently, we design a catalyst with more Au + sites, which exhibits enhanced catalytic activity. This work systematically elucidates the structure–activity relationship and provides a promising strategy to optimize SACs for the hydrodeoxygenation reaction.

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 head0.030
GPT teacher head0.251
Teacher spread0.220 · 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

Citations27
Published2023
Admission routes1
Has abstractyes

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