A Redox-Active Frustrated Lewis Pair for the Activation and N–O Scission of Nitrosonium Cations
Bibliographic record
Abstract
Frustrated Lewis pairs (FLPs) have revolutionized main-group chemistry by enabling reactivity traditionally associated with transition metals. However, existing FLP systems are predominantly restricted to two-electron heterolytic or homolytic bond activation mechanisms. In this work, we present a phosphine functionalized with a peripheral redox-active phenothiazine moiety and explore its unique behavior within an FLP framework. The resulting FLP exhibits unprecedented reactivity, allowing for the activation of the highly oxidizing nitrosonium cation with subsequent N-O bond scission. This reaction is facilitated by the redox-active functionality, first being oxidized by a single electron, then producing a reactive FLP that activates NO, resulting in an overall 3-electron bond activation. This novel transformation underscores the potential of incorporating redox-active groups to expand the scope of FLP chemistry, paving the way for new avenues in main-group bond activations.
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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".