Local Modulation of Single-Atomic Mn Sites for Enhanced Ambient Ammonia Electrosynthesis
Why this work is in the frame
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Bibliographic record
Abstract
Rationally tuning the local structures of single-atomic active sites for the electrocatalytic N2 reduction reaction (NRR) remains an urgent but worthwhile research topic. Herein, we accomplish the local modulation of single-atomic Mn sites and construct single Mn–O3N1 sites anchored on porous carbon (Mn–O3N1/PC) by delicately controlling the Mn–O bonding conditions. The constructed structures are confirmed via the combination of atomic-scale imaging, Raman spectroscopy, synchrotron radiation-based soft and hard X-ray absorption spectroscopies, and X-ray photoelectron spectroscopy. The Mn–O3N1/PC catalyst yields an NH3 yield rate of 66.41 μg h–1 mgcat.–1 (corresponding to 1.56 mg h–1 mgMn–1) at −0.35 V versus reversible hydrogen electrode, which is about four times that on the control Mn–N4/PC catalyst. The enhanced NRR performance is ascribed to its unique geometry and electronic structures, which not only facilitate the adsorption and activation of the N2 molecule but also lower the free energy change of the potential-determining step.
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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 | 0.000 | 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 it