Rational design of palladium single-atoms and clusters supported on silicoaluminophosphate-31 by a photochemical route for chemoselective hydrodeoxygenation of vanillin
Bibliographic record
Abstract
Chemoselective hydrodeoxygenation of vanillin is of great importance in converting biomass into high value-added chemicals. Herein, we describe a facile photochemical route to access palladium single atoms and clusters supported on silicoaluminophosphate-31 (SAPO-31) as a highly active, chemoselective, and reusable catalyst for hydrodeoxygenation of vanillin. Characterizations by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy, extended X-ray absorption fine structure measurement, and CO-absorbed diffuse reflectance infrared Fourier transform spectroscopy reveal the atomically dispersed palladium single atoms and clusters are loosely bonded and randomly dispersed, without forming strong palladium-palladium metallic bonding, over the SAPO-31 support. This catalyst, with a full metal availability to the reactants, exhibits exceptional catalytic activity (TOF: 3,000 h−1, Yield: > 99%) in the hydrodeoxygenation of vanillin toward 2-methoxy-4-methylphenol (MMP) under mild conditions (1 atm, 80 °C, 30 min), along with excellent stability, scalability (up to 100-fold), and wide substrate scope. The superior catalytic performance can be attributed to the synergistic effect of the positively charged palladium single atoms and fully exposed clusters, as well as the strong metal-support interactions. This work may offer a new avenue for the design and synthesis of fully exposed metal catalysts with targeted functionalities.
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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".