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Crystallographic identification of a novel 2,4,5-tri(N-methyl-4-pyridinium)-1,3-thiazole with a complex network of polyiodide/iodine counter ions and co-crystallized cyclododecasulfur (S12)

2021· article· en· W3175410027 on OpenAlexafffund
Ibukun Oluwaseun Shotonwa, Renè T. Boeré

Bibliographic record

VenueEuropean Journal of Chemistry · 2021
Typearticle
Languageen
FieldChemistry
TopicCrystal structures of chemical compounds
Canadian institutionsUniversity of Lethbridge
FundersNatural Sciences and Engineering Research Council of CanadaUniversity of Lethbridge
KeywordsChemistryMonoclinic crystal systemCrystallographyLattice energyThiazoleCrystal structureIodideTriiodideHydrogen bondThioamideCrystal (programming language)PyridiniumTetragonal crystal systemMoleculeStereochemistryInorganic chemistryPhysical chemistryOrganic chemistry

Abstract

fetched live from OpenAlex

The crystals of an unprecedented 2,4,5-tri(N-methylpyridinium)-1,3-thiazole are monoclinic and belong to the space group P21/c as determined by single-crystal XRD. Crystal data for C21H21I13N4S5.98: monoclinic, a = 7.5627(5) Å, b = 30.6764(19) Å, c = 20.8848(15) Å, β = 91.632(6)°, V = 4843.2(6) Å3, Z = 4, T = 100.01(10) K, μ(Cu Kα) = 67.840 mm-1, Dcalc = 2.977 g/cm3, 17906 reflections measured (7.152° ≤ 2Θ ≤ 162.94°), 17906 unique (Rsigma = 0.0607) which were used in all calculations. The final R1 was 0.1366 (I > 2σ(I)) and wR2 was 0.3926 (all data). The crystal lattice contains 2,4,5-tri(N-methylpyridinium)-1,3-thiazole, molecular iodine and triiodide counterions which interact with one another to coordinatively form polyiodides, as well as a surprising co-crystallized neutral molecule of cyclododecasulfur (S12). Close monitoring of the synthetic procedure reveals chemical condensation and decomposition of the thioamide reagent to be the impetus for the formation of individual components of the crystal lattice. Analysis of the XRD, including a Hirshfeld surface analysis, shows that (a) the crystal lattice has a number of stabilizing Coulombic short contacts such as I∙∙∙I, I∙∙∙S, I∙∙∙C, and C∙∙∙S and non-classical C-H∙∙∙I and C-H∙∙∙S hydrogen bond interactions (b) the iodine/iodide network are major determinants in the stability of its crystal lattice despite the reduced occupancies of sulfur and (c) the Hirshfeld analysis in comparison with the conventional Mercury visualization program was able to simplify, identify and quantify complex atom-atom interactions such as H∙∙∙H and N∙∙∙I in its crystal lattice. Herein, it is reported, for the first time, the formation of co-crystallized, neutral cyclododecasulfur (S12) from thioamide as the sulfur source. S12 displays a consistent geometry and comparable average S-S distances, S-S-S angles and torsion angles with previously reported crystal structures of S12. The complex network facilitated by the formation of polyiodides via the interaction of symmetric and asymmetric triiodides and iodine has resulted in quite strong interactions that are less than the sums of the van der Waals radii of two connected atoms as well as an array of fascinating geometrical alignments such as T-shape, trigonal pyramidal and L-shape.

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 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 score0.015
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.000
Science and technology studies0.0000.001
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0000.001
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 head0.015
GPT teacher head0.239
Teacher spread0.224 · 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".

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Citations0
Published2021
Admission routes2
Has abstractyes

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