Screening Single-Atom-Doped Transition Metal CuFe Alloy Catalysts for Electrochemical Urea Synthesis
Bibliographic record
Abstract
Electrochemical C–N coupling offers a sustainable route for the synthesis of urea from CO 2 and N 2 . However, it is challenged by the scarcity of active and highly selective catalysts. In this study, we present a rational strategy to design transition metal (TM)-doped single-atom alloy (SAA) electrocatalysts. We investigated a CuFe bimetallic alloy as a host to enable facile coactivation of CO 2 and N 2 . Through a multistep process using quantum mechanical calculations, 3d, 4d, and 5d TM dopants on the CuFe surface were screened to assess catalyst synthesizability, activity, and selectivity against competing pathways, including hydrogen evolution reaction, ammonia formation, and C 2 product formation. Among all TMs, Ti, Cr, Mo, and W were identified as promising candidates that can form thermodynamically stable SAAs in the CuFe bimetallic alloy. W-doped CuFe emerged as the most selective and favorable candidate for urea production, and the electronic structure analysis revealed the origin of the high selectivity. While Cr and Ti catalysts showed overbinding due to high d-band centers, strong hybridization, and excessive charge transfer, the W dopant achieves an optimal electronic balance, enabling controlled back-donation to both N 2 and CO 2 molecules, facilitating dual activation. Mechanistic investigation revealed the reaction pathway involving a C–N coupling step to form the *NCON intermediate, with an activation free-energy barrier of 1.08 eV on W SAA. Cr, Mo, and Ti were relatively less active and selective. This work presents a rational strategy for designing SAAs for targeted C–N bond formation.
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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".