Structurally Disordered Phosphorus-Doped Pt as a Highly Active Electrocatalyst for an Oxygen Reduction Reaction
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Bibliographic record
Abstract
The application of Pt alloy catalysts for oxygen reduction reactions (ORRs) in proton-exchange membrane fuel cells is severely impeded by base metal leaching, since the produced metal ions can result in the degradation of a Nafion membrane by replacing H+ and inducing a Fenton reaction. Doping Pt with nonmetal elements can significantly mitigate such problems due to the relative harmlessness of the corrosion products of anions. Herein, we developed a phosphorus-doping strategy, which can greatly boost the ORR performance of Pt. Phosphorus was introduced into the near-surface of commercial Pt/C (denoted as PNS-Pt/C) via a surfactant-free method. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray photoelectron spectrum (XPS) tests indicate that the introduction of phosphorus induced distortion of the Pt lattice and the downshift of the d-band center. In situ electrochemical Fourier transform infrared (FTIR) spectroscopy with adsorbed CO as a molecule probe further revealed that the introduction of phosphorus can lower the adsorption ability. The ORR mass activity of PNS-Pt/C is as high as 1.00 mA μgPt–1@0.90 V, which is enhanced by 7 times in comparison with the initial Pt/C catalyst. Meanwhile, the durability is also enhanced. After 10 000 potential cycles, PNS-Pt/C only lost 14% of the ORR mass activity, while Pt/C lost 51%. More importantly, a H2–air fuel cell with a PNS-Pt/C cathode achieves a power density of 1.06 W cm–2 at a current density of 2.0 A cm–2 with a low Pt loading of 0.15 mg cm–2. The current density at 0.60 V (practical working potential) is 1.54 A cm–2, 2 times higher than that of commercial Pt/C. Density functional theory (DFT) calculations indicate that near-surface phosphorus doping can induce the distortion of the Pt surface, on which some concave Pt sites have optimal binding energy of OH for the ORR. Furthermore, this phosphorus-doping strategy is also valid for a PtNi alloy catalyst to further boost the ORR performance.
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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) | 0.001 | 0.001 |
| Meta-epidemiology (broad) | 0.001 | 0.000 |
| Bibliometrics | 0.000 | 0.001 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.001 |
| Open science | 0.001 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| 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 it