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 machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| 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) | 0.001 | 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 source (direct Gemma or distilled Codex), 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".