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Record W4308271435 · doi:10.26434/chemrxiv-2022-w9qvx

Planar Bismuth Triamides: A Tunable Platform for Main Group Lewis Acidity and Polymerization Catalysis

2022· preprint· en· W4308271435 on OpenAlexafffund
Tyler J. Hannah, W. Michael McCarvell, Tamina Kirsch, Toren Hynes, Jacqueline Mayho, Karlee L. Bamford, Cyler W. Vos, Christopher M. Kozak, Tanner George, Jason D. Masuda, Saurabh S. Chitnis

Bibliographic record

VenueChemRxiv · 2022
Typepreprint
Languageen
FieldChemistry
TopicOrganoboron and organosilicon chemistry
Canadian institutionsMemorial University of NewfoundlandWestern UniversityDalhousie University
FundersNatural Sciences and Engineering Research Council of CanadaDalhousie UniversityYork University
KeywordsChemistryLewis acids and basesBismuthCatalysisSteric effectsPolymerizationLigand (biochemistry)Computational chemistryCombinatorial chemistryPolymer chemistryOrganic chemistryPolymer

Abstract

fetched live from OpenAlex

Geometric deformation in main group compounds can be used to elicit unique properties including strong Lewis acidity. Here we report on a family of planar bismuth (III) complexes (c.f. typically pyramidal structure for such compounds), which show a geometric Lewis acidity that can be further tuned by varying the steric and electronic features of the triamide ligand employed. The structural dynamism of the planar bismuth complexes was probed in both the solid and solution phase, revealing at least three distinct modes of intermolecular association. A modified Gutmann-Beckett method was used to assess their electrophilicity by employing trimethylphosphine sulfide in addition to triethylphosphine oxide as probes, providing insights into the preference for binding hard or soft substrates. Experimental binding studies were complemented by a computational assessment of the affinities and dissection of the latter into their intrinsic bond strength and deformation energy components. The results show comparable Lewis acidity to triarylboranes, with the added ability to bind two bases simultaneously and reduced discrimination against soft substrates. We also study the catalytic efficacy of these complexes in the ring opening polymerization of cyclic esters ε-caprolactone and rac-lactide. The polymers obtained are in the ultra-high molecular weight regime and show excellent dispersity values. The complexes retain their performance under industrially relevant conditions suggesting they may be useful as less toxic alternatives to tin catalysts in the production of medical grade materials. Collectively, these results establish planar bismuth complexes as not only a novel neutral platform for main group Lewis acidity, but also a potentially valuable one for catalysis.

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 score0.003

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 head0.021
GPT teacher head0.245
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 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

Citations0
Published2022
Admission routes2
Has abstractyes

Explore more

Same venueChemRxiv→Same topicOrganoboron and organosilicon chemistry→French-language works237,207→