Unusual Sabatier principle on high entropy alloy catalysts for hydrogen evolution reactions
Bibliographic record
Abstract
Abstract The Sabatier principle is widely explored in heterogeneous catalysis, graphically depicted in volcano plots. The most desirable activity is located at the peak of the volcano, and further advances in activity past this optimum are possible only by designing a catalyst that circumvents the limitations entailed by the Sabatier principle. In this work, by density functional theory calculations, we found that high entropy alloy (HEA) surface with spatially varying adsorption free energy of hydrogen (ΔGH*), where the active sites with strong adsorption adsorb hydrogen (H*) and other sites with weak adsorption release H* to produce H2, was against the “just right” (ΔGH* = 0 eV) in the Sabatier principle of hydrogen evolution reaction (HER). The Gaussian distribution [X ~ N(µ, σ2)] of ΔGH* on HEA was proposed as a descriptor, deriving an anomalous Sabatier principle, where a larger σ value results with µ = 0 eV results in a higher catalytic activity for HER. As a proof-of-concept, we synthesized a series of alloy systems, the PtFeCoNiCu HEA catalyst has the best catalytic performance for HER with an overpotential of 10.8 mV at -10 mA cm− 2 and 4.6 times higher intrinsic activity over the state-of-the-art Pt/C. Moreover, the calculated adsorption energy of C*, O*, and N* on HEAs also follows a Gaussian distribution, indicating the anomalous Sabatier principle can be extended to other related catalytic reactions.
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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".