Fe−N<sub>3</sub>/C Active Catalytic Sites for the Oxygen Reduction Reaction Prepared with Molecular‐Level Geometry Control through the Covalent Immobilization of an Iron−Terpyridine Motif onto Carbon
Bibliographic record
Abstract
Abstract A model for a non‐precious metal catalyst for the oxygen reduction reaction (ORR) in aqueous media has been prepared by functionalizing a commercial Vulcan XC‐72 carbon support with a terpyridine‐based nitrogenous ligand. The terpyridine ligand geometry allows the formation of active catalytic sites by selectively embedding a N 3 /C structural motif into the carbon support confirmed by using thermogravimetric analysis (TGA) and X‐ray photoelectron spectroscopy (XPS) measurements. Room‐temperature metal–ligand coordination results in the desired Fe−N 3 /C moieties on the surface. This model system was used to demonstrate the catalytic activity of the surfaces containing mainly Fe−N 3 sites for the ORR in acidic and basic media. Importantly, we demonstrate that the system could be prepared under mild reaction conditions, does not require high‐ temperature treatments, and shows catalytic activity for the ORR. Interestingly, when the system was pyrolyzed in an N 2 atmosphere at 700 °C the resulting activity declined. The non‐heat‐treated Fe−N 3 /C surface demonstrates comparable activity in acidic electrolyte medium when compared to most literature catalysts that are typically heat treated to produce four nitrogen atoms coordinated to one iron center (Fe−N 2+2 /C). Interestingly, despite the fact that many systems reported so far in the literature exhibit enhanced activity after heat treatment, our system showed an increase in activity when the material was not pyrolyzed.
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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 | 0.001 |
| 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) | 0.000 | 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".