Highly Accessible Electrocatalyst with <i>I</i><i>n Situ</i> Formed Copper-Cluster Active Sites for Enhanced Nitrate-to-Ammonia Conversion
Bibliographic record
Abstract
Ammonia synthesis via nitrate electroreduction is more attractive and sustainable than the energy-extensive Haber–Bosch process and intrinsically sluggish nitrogen electroreduction. Herein, we have designed a single-site Cu catalyst on hierarchical nitrogen-doped carbon nanocage support (Cu 1 /hNCNC) for nitrate electroreduction, which achieves an ultrahigh ammonia yield rate (YR NH3 ) of 99.4 mol h –1 g Cu –1 (2.30 mol h –1 g cat. –1 ) with ammonia Faradaic efficiency (FE NH3 ) of 99.3%, far beyond the most reported single-site catalysts on carbon-based supports. The combined operando characterization and theoretical studies indicate that the in situ formed Cu-cluster active sites are responsible for the high YR NH3 and FE NH3 due to the enhanced NO 3 – adsorption and subsequent protonation on the unique Cu 3 –N 4 moieties, and meanwhile, the hierarchical hNCNC support facilitates the mass/charge transfer kinetics, thus promoting the high expression of intrinsic activity. The demonstration of plasma N 2 oxidization and nitrate electroreduction cascade reaction manifests the great potential of the Cu 1 /hNCNC electrocatalyst in sustainable NH 3 synthesis. These findings offer valuable insights into the design of effective catalysts for electrosynthetic reactions.
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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".