Dynamic reversible evolution of vicinal/bonding heteronuclear diatoms drives relay reductive C–N coupling for enhancive urea electrosynthesis
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Bibliographic record
Abstract
Abstract The precise construction of dual active sites has been uncovered for the electroreduction of C‐ and N‐based precursors to synthesize urea. However, these strategies often face adsorption scaling constraints and spatial restrictions that hinder C–N coupling, resulting in suboptimal activity and selectivity. Here, we showcase a dynamically reversible evolution between vicinal Fe/Cu diatoms and alloy‐like Fe–Cu sites, enabling cascade protonation and efficient C–N coupling. This approach markedly enhances urea electrosynthesis from CO 2 and NO 3 − , achieving an ultrahigh urea yield of 2421.2 μg h −1 mg −1 , Faraday efficiency (FE) of 70.4%, and C‐selectivity of 96.7%, surpassing state‐of‐the‐art dual‐site electrocatalysts. Operando spectroscopy and theoretical calculations reveal that neighboring Fe/Cu diatoms facilitate the selective adsorption and hydrogenation of NO 3 − and CO 2 into the key intermediates (*NO and *CO). Furthermore, alloy‐like Fe–Cu sites, formed in situ due to declined metal surface free energy driven by electron transfer, facilitate C–N coupling and subsequent protonation to selectively produce urea, while dynamically reverting to vicinal Fe/Cu diatoms. This work provides new insights into the relay catalytic strategy for urea electrosynthesis by modulating the dynamic atomic‐scale evolution of active sites. image
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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)
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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