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Record W4391092140 · doi:10.1021/acs.chemmater.3c02288

Enantiopure Chiral Au<sub>13</sub> Nanoclusters Stabilized by Ditopic <i>N</i>-Heterocyclic Carbenes: Synthesis, Characterization, and Electrocatalytic Reduction of CO<sub>2</sub>

2024· article· en· W4391092140 on OpenAlexafffund
Emily L. Albright, Sami Malola, Samuel I. Jacob, Hong Yi, Shinjiro Takano, Koichi Mimura, Tatsuya Tsukuda, Hannu Häkkinen, Masakazu Nambo, Cathleen M. Crudden

Bibliographic record

VenueChemistry of Materials · 2024
Typearticle
Languageen
FieldMaterials Science
TopicNanocluster Synthesis and Applications
Canadian institutionsQueen's University
FundersSocial Sciences and Humanities Research Council of CanadaNatural Sciences and Engineering Research Council of CanadaResearch Foundation for the Electrotechnology of ChubuAmerican Chemical Society Petroleum Research FundJapan Society for the Promotion of ScienceMinistry of Education, Culture, Sports, Science and TechnologyCanada Foundation for Innovation
KeywordsNanoclustersChemistryEnantiopure drugEnantiomerChirality (physics)Circular dichroismCrystallographyElectrospray ionizationDensity functional theorySuperatomMass spectrometryStereochemistryComputational chemistryEnantioselective synthesisOrganic chemistryCatalysis

Abstract

fetched live from OpenAlex

A series of chiral Au 13 nanoclusters were synthesized via the direct reduction of chiral dinuclear Au(I) halide complexes ligated by chiral dioxalone-linked bis- N -heterocyclic carbene (bisNHC) ligands. Electrospray ionization mass spectrometry, nuclear magnetic resonance spectroscopy, and density functional theory (DFT) calculations confirmed the molecular formula to be [Au 13 (bisNHC) 4 I 4 ] +, with a chiral arrangement of the four ditopic NHC ligands around the icosahedral Au 13 core. Circular dichroism (CD) spectroscopy of the two enantiomers of the Au 13 clusters shows distinct mirror images of the enantiomers and supports chirality transfer from ligands to the metal core. A plausible model structure was built with the assistance of theoretical analysis, and DFT calculations were employed to explain the origin of the optical and CD activities and their dependence on the binding arrangement of the ditopic bisNHC ligands. The clusters show remarkable stability with minimal decomposition in various solutions both at elevated and room temperatures. The potential of these clusters as nanocatalysts in the electrocatalytic reduction of CO 2 to CO is described.

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)0.000
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow)
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 score0.002
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
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)0.0000.000

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 head0.215
Teacher spread0.208 · 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

Citations24
Published2024
Admission routes2
Has abstractyes

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