Ligand Effects and Kinetic Investigations of Sterically Accessible 2-Pyridonate Tantalum Complexes for Hydroaminoalkylation
Bibliographic record
Abstract
The synthesis of a series of structurally varied pyridonate-supported tantalum amido complexes and their catalytic reactivity in the intermolecular α-alkylation of unprotected secondary amines are described. Both terminal and internal alkenes can undergo this hydroaminoalkylation reaction to give selectively substituted secondary amine products. The reactivity profiles of 3- and 6-substituted pyridonate tantalum complexes, [(2-pyridonate)Ta(NMe 2 ) 3 Cl], and a triflato pyridonate tantalum complex, [(2-pyridonate)Ta(NMe 2 ) 3 OTf], were evaluated to analyze ligand effects. The deprotonation and complexation of commercially available 3-methyl-2-pyridone and 2-pyridone readily yielded effective, catalytically active tantalum complexes, displaying reactivity with both terminal and internal alkene substrates. Kinetic studies and deuterium labeling experiments reveal a complex kinetic profile and provide evidence for off-cycle equilibria that dominate catalytic activity and provide guidance for future catalyst development.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot 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.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.001 | 0.000 |
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.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.
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".