Sequential hydrogenation enhanced by bidirectional hydrogen spillover over cascade catalyst
Bibliographic record
Abstract
Abstract Formulating a synergetic strategy to govern the catalytic function of dual metal sites is paramount to achieving precise control of cascade reactions. Herein, we construct a dual‐site cascade catalyst with Pt and Ru species localized in the micropores and mesopores of zeolite, respectively. This architecture enables the spatial separation of Pt and Ru sites in nanoscale proximity. Compared to mono/bi‐metallic catalysts, this cascade catalyst enables a 4.4–9.5 times enhancement in activity during the sequential hydrogenation of nitroaromatics to cyclohexylamine. Particularly, bidirectional hydrogen spillover assists hydrogenation between Pt and Ru sites is confirmed, where active hydrogen migrates from the less catalytic activity metal to the adjacent metal sites during the first/second step in the cascade reaction. Characterization studies and density functional theory calculations suggest that bidirectional hydrogen spillover enhances the coverage of active hydrogen at the active sites for each hydrogenation step, thereby reducing the energy barrier of the rate‐controlling step. This intriguing phenomenon reveals the mechanism of accelerated hydrogenation and presents an opportunity for devising immensely efficient cascade catalysts.
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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) | 0.003 | 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".