Pd 4d Orbital Overlapping Modulation on Au@Pd Nanowires for Efficient H<sub>2</sub>O<sub>2</sub> Production
Bibliographic record
Abstract
Isolating Pd atoms has been shown to be crucial for the design of a Pd-based electrocatalyst toward 2e – oxygen reduction reaction (ORR). However, there are limited studies focusing on the systematic compositional design that leads to an optimal balance between activity and selectivity. Herein, we design a series of Au@Pd core@shell structures to investigate the influence of the Pd 4d orbital overlapping degree on 2e – ORR performance. Density functional theory (DFT) calculations indicate that enhanced H 2 O 2 selectivity and activity are achieved at Pd n clusters with n ≤ 3, and Pd clusters larger than Pd 3 should be active for 4e – ORR. However, experimental results show that Au@Pd nanowires (NWs) with Pd 4 as the primary structure exhibit the optimal H 2 O 2 performance in an acidic electrolyte with a high mass activity (7.05 A mg –1 at 0.4 V) and H 2 O 2 selectivity (nearly 95%). Thus, we report that Pd 4, instead of Pd 3, is the upper threshold of Pd cluster size for an ideal 2e – ORR. It results from the oxygen coverage on the catalyst surface during the ORR process, and such an oxygen coverage phenomenon causes electron redistribution and weakened *OOH binding strength on active sites, leading to enhanced activity of Pd 4 with only 0.06 V overpotential in acidic media.
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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 | 0.001 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.001 |
| Bibliometrics | 0.000 | 0.001 |
| 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) | 0.000 | 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".