Electrochemically Driven C-N Bond Formation from CO2 and Ammonia at the Triple-Phase Boundary
Bibliographic record
Abstract
Electrosynthetic techniques are gaining prominence across the fields of chemistry, engineering and energy science. However, most works within the direction of synthetic heterogeneous electrocatalysis focus on water electrolysis and CO 2 reduction. In this work, we moved to expand the scope of this technology by developing a synthetic scheme which couples CO 2 and NH 3 at a gas-liquid-solid triple-phase boundary to produce species with C-N bonds. Specifically, by bringing in CO 2 from the gas phase and NH 3 from the liquid phase together over solid copper catalysts, we have succeeded in forming formamide and acetamide products for the first time. In a subsequent complementary step, we have combined electrochemical analysis and a newly developed operando spectroelectrochemical method, capable of probing the aforementioned triple phase boundary, to extract an initial level of mechanistic analysis regarding the reaction pathways of these reactions and the current system’s limitations. We believe that the development and understanding of this set of reaction pathways will play an exceptionally significant role in expanding the community’s understanding of on-surface electrosynthetic reactions as well as push this set of inherently sustainable technologies towards widespread applicability.
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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 | 0.001 |
| 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".