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Record W4405570479 · doi:10.1021/acs.inorgchem.4c04503

Trends in Methanol-Solvated Actinide Ions and Actinide Expanded Porphyrin Complexes

2024· article· en· W4405570479 on OpenAlexafffund
Meagan S. Oakley, Georg Schreckenbach

Bibliographic record

VenueInorganic Chemistry · 2024
Typearticle
Languageen
FieldChemistry
TopicRadioactive element chemistry and processing
Canadian institutionsUniversity of Manitoba
FundersNatural Sciences and Engineering Research Council of CanadaUniversity of ManchesterAlliance de recherche numérique du CanadaWestern Canada Research Grid
KeywordsChemistryActinidePorphyrinLanthanideDensity functional theoryBinding energyInorganic chemistryComputational chemistrySolvationIonCrystallographyPhysical chemistryPhotochemistryOrganic chemistryAtomic physics

Abstract

fetched live from OpenAlex

Trivalent actinide expanded porphyrin complexes have been of synthetic interest since the isolation of the series of trivalent lanthanide texaphyrin complexes in 1992, however, synthesis of these actinide-based complexes has not yet been achieved. In this work, a computational study with relativistic density functional theory was performed to determine how trivalent actinide ions (Ac 3+ through Lr 3+ ) interact with Schiff base expanded porphyrin macrocycles in a methanol solvent as an alternate pathway to stabilization. A thorough analysis of structural parameters, electronic structure, stability of microsolvation environments, and relative binding energies provided insight into the most stable structures. Trends in bonding and structure for the full actinide series are reported for methanol solvated ions, which reports actinide contraction along the series for early and mid actinides. Texaphyrin incorporates the actinide ions in a planar fashion, whereas for alaskphyrin a bent structure is more favorable; this bend results in stronger interaction energies than those calculated for the texaphyrin complexes. We also show that the redox-active expanded porphyrin ligands are able to accommodate a variety of actinides through charge transfer stabilization. Based on relative binding energy and energy decomposition analysis, it was found that texaphyrin and alaskaphyrin both exhibit a strong preference for binding to Th.

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 score0.002
Threshold uncertainty score0.006

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)0.0020.000

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 head0.019
GPT teacher head0.285
Teacher spread0.266 · 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

Citations2
Published2024
Admission routes2
Has abstractyes

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