Regulating second-shell coordination in molybdenum single-atom catalysts for efficient photocatalytic nitrogen fixation
Bibliographic record
Abstract
• A novel molybdenum single-atom catalysts with boron coordinated in the second shell was developed. • Mo SAs/BCN exhibited superior visible-light-driven photocatalytic activity for N 2 reduction to NH 3 . • The relationship between NRR performance and local coordination structure was clarified. • The N 2 reduction pathways on Mo SAs/BCN was elucidated. Photocatalytic nitrogen (N 2 ) reduction reaction (NRR) holds great potential and sustainability compared with the Haber-Bosch process for ammonia (NH 3 ) synthesis. Precise regulation of the coordination environment in the second shell of single-atom catalysts (SACs) provides an opportunity to enhance the photocatalytic NRR performance, yet a challenge. Herein, Mo SAs/BCN featured by Mo single atoms dispersed in a carbon nitride support with second-shell B coordination is developed for photocatalytic N 2 fixation. Experimental data combined with theoretical calculations demonstrate that the second-shell B coordination can not only strengthen visible light absorption and accelerate the separation and transfer of photogenerated charge carriers, but also upshift the d-band center of Mo close to the Fermi level to improve the adsorption and activation of N 2 . Thus, Mo SAs/BCN exhibits a high NH 3 yield rate of 176.4 μmol g -1 cat. h −1 under visible light irradiation, which is 5.4 times that of CN. A distal pathway may occur on Mo SAs/BCN, and the first step of *N 2 protonation is the potential-determination step. This work reveals the significance of modulating the second-shell coordination atoms of SACs for enhancing photocatalytic activity and selectivity and offers a promising strategy for the rational design of SACs.
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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 | 0.000 | 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".