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Record W2036198777 · doi:10.1021/ic5000183

Site-Selective High-Resolution X-ray Absorption Spectroscopy and High-Resolution X-ray Emission Spectroscopy of Cobalt Nanoparticles

2014· article· en· W2036198777 on OpenAlex
Timna‐Josua Kühn, J. Hormes, Nina Matoussevitch, Helmut Bönnemann, Pieter Glatzel

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

VenueInorganic Chemistry · 2014
Typearticle
Languageen
FieldPhysics and Astronomy
TopicX-ray Spectroscopy and Fluorescence Analysis
Canadian institutionsCanadian Light Source (Canada)University of Saskatchewan
FundersEuropean Synchrotron Radiation Facility
KeywordsX-ray absorption spectroscopyChemistryXANESAbsorption spectroscopyExtended X-ray absorption fine structureAnalytical Chemistry (journal)Emission spectrumSpectroscopySpectral lineNanoparticleAbsorption (acoustics)X-ray spectroscopySynchrotron radiationMaterials scienceNanotechnologyOpticsPhysics

Abstract

fetched live from OpenAlex

The special (macroscopic) properties of nanoparticles are mainly due to their large surface-to-volume ratio. Thus, the separate characterization of geometric and electronic properties of surface and bulk would be favorable for a better understanding of the properties of nanoparticles. Because of the chemical sensitivity of X-ray fluorescence lines, in particular those involving higher lying electronic states, high-resolution fluorescence-detected X-ray absorption spectra (HRFD-XAS) offer these opportunities. In this study, three types of wet-chemically synthesized Co nanoparticles, ∼6 nm in diameter with varying thicknesses of a protective shell, were investigated at the ID26 beamline of the European Synchrotron Radiation Facility. HRFD-XAS spectra at the Co K-edge, that is, X-ray absorption near-edge structure (HRFD-XANES) and extended X-ray absorption fine structure (HRFD-EXAFS) spectra, were recorded via detection of the Kβ1,3 fluorescence at specific energies. As these spectra are only partly site-selective due to a strong overlap of the emission lines, a numerical procedure was applied based on a least-squares fitting procedure, realized by singular value decomposition. The detailed analysis of the obtained site-selective spectra, regarding chemical composition and crystallographic phase, using measured and simulated FEFF9-based reference spectra, showed that the metallic core had mainly hexagonal close-packed structure with lattice constants matching bulk Co; the spectra for the shell could be satisfactorily fitted by a mixture of CoO and CoCO3; however, with an obvious need for at least a third compound. To obtain additional information about ligands attached to Co, valence-to-core X-ray emission spectra (VTC-XES) using the Kβ2,5 and the satellite structure Kβ″ and VTC-XANES spectra thereof were also recorded, by which the former results are confirmed. Further on, FEFF simulations indicate that a Co-N compound is a very likely candidate for the third component. The presented results clearly show that VTC-XES and HRFD-XAS are suitable tools for the detailed specification of the core and the surface of nanoparticles, in particular upon realizing "real" site-selectivity for XANES and EXAFS with a general strategy applicable to a wide range of systems.

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 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 score0.013
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
Bibliometrics0.0000.001
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 head0.004
GPT teacher head0.216
Teacher spread0.212 · 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