Manipulating Reactivity of Ir(CH<sub>2</sub>)<sub>0–2</sub><sup>+</sup> Cations toward Dinitrogen at Room Temperature: A Unique Dependence on the Organic Ligand Structures
Bibliographic record
Abstract
Nitrogen (N 2 ) activation at room temperature has long been a great challenge. Therefore, the rational design of reactive species to adsorb N 2, which is a prerequisite for cleavage of the strong N≡N triple bond in industrial and biological processes, is highly desirable and meaningful. Herein, the N 2 adsorption process is controlled by regulating the types and numbers of organic ligands, and the organic ligands are produced through the reactions of Ir + with methane and ethane. CH 4 molecules dissociate on the Ir + cations to form Ir(CH 2 ) 1,2 + . The reaction of Ir + with C 2 H 6 can generate HIrC 2 H 3 +, which is different from the structure of Ir(CH 2 ) 2 + obtained from Ir + /CH 4 . The reactivity order of N 2 adsorption is Ir(CH 2 ) 2 + > HIrC 2 H 3 + ≫ HIrCH + ≈ Ir + (almost inert under similar reaction conditions), indicating that different organic ligand structures affect reactivity dramatically. The main reason for this interesting reactivity difference is that the lowest unoccupied molecular orbital (LUMO) level of Ir(CH 2 ) 2 + is much closer to the highest occupied molecular orbital (HOMO) level of N 2 than those of the other three systems. This study provides new insights into the adsorption of N 2 on metal–organic ligand species, in which the organic ligand dominates the reactivity, and it discovers new clues in designing effective transition metal carbine species for N 2 activation.
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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot 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.
Codex and Gemma teacher scores by category
| 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 | 0.001 | 0.000 |
| Research integrity | 0.000 | 0.001 |
| Insufficient payload (model declined to judge) | 0.000 | 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 teacher head, 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".