Revealing the structure-activity relationship of Pt1/CeO2 with 17O solid-state NMR spectroscopy and DFT calculations
Bibliographic record
Abstract
Single-atom catalysts (SACs) have attracted significant interest due to their exceptional and tunable performance, enabled by diverse coordination environments achieved through innovative synthetic strategies. However, various local structures of active sites pose significant challenges for precise characterization, a prerequisite for developing structure-activity relationships. Here, we combine 17O solid-state NMR spectroscopy and DFT calculations to elucidate the detailed structural information of Pt/CeO2 SACs and their catalytic behaviors. The NMR data reveal that single Pt atoms, dispersed from clusters with water vapor, exhibit a square planar geometry embedded in CeO2 (111) surface, distinct from the original clusters and other conventionally generated Pt single atoms. The square planar Pt/CeO2 SAC demonstrates improved CO oxidation performance compared to Pt/CeO2 SAC with octahedral coordination, due to moderately strong CO adsorption and low energy barriers. This approach can be extended to other oxide-supported SACs, enabling spatially resolved characterization and offering comprehensive insights into their structure-activity relationships. Properly characterising active sites in single atom catalysts is important for mechanistic understanding but remains difficult. Here the authors combine 17O solid-state NMR spectroscopy and DFT calculations to probe the structures of Pt/CeO2 single atom catalysts, gaining insights into their structure-activity relationships.
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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 | 0.001 |
| Science and technology studies | 0.001 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.001 | 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".