<i>In Situ</i> Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy Study of Nickel Surface Oxides Reveals Previously Unseen Surface Chemical Dynamics
Bibliographic record
Abstract
High Resolution Image Download MS PowerPoint Slide Potential-dependent shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) is applied to study the surface oxide/hydroxide formation and reduction on a planar polycrystalline Ni electrode surface in contact with alkaline aqueous solutions. A new Raman amplifier, stable in alkaline aqueous solutions, is fabricated by introducing a thin layer of ZrO 2 on the surface of Au nanoparticles (NPs). The thickness of the ZrO 2 layer is controlled to be 2–3 nm, so the resulting ZrO 2 -modified Au NPs selectively enhanced the Raman signals of the surface oxide/hydroxide species, with the amplifiers remaining spectroscopically silent. In situ SHINERS measurements were combined with electrochemical measurements. Potential-dependent Raman signals from the thin layer of surface oxides/hydroxides, namely, α-Ni(OH) 2, β-Ni(OH) 2, β-Ni(O)OH, γ-Ni(O)OH, and Ni-OO – species, are successfully identified in the potential range between the onsets of the hydrogen and oxygen evolution reactions (HER, OER). The combined SHINERS and electrochemical measurements shed new light on the chemical identity of Ni surface oxide/hydroxide species and their potential-driven interconversions. In particular, the transformations of surface species, such as α-Ni(OH) 2 to β-Ni(OH) 2 and γ-Ni(O)OH to β-Ni(O)OH, which had not been described in voltammograms, were identified in the spectral behavior. The measurements also enable the identification of the precursor of the OER; thus SHINERS can be useful in establishing a correlation between the chemical state of the Ni electrode and the OER activity, the slowest electrode process occurring in alkaline water electrolyzers, emphasizing the importance of this technique to the development of electrocatalysts. The SHINERS and electrochemical results are supported by density functional theory (DFT) calculations. The outcome of this research results in an updated Bode scheme for the electrochemical oxidation products of Ni materials in aqueous alkaline 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 | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.001 | 0.000 |
| Bibliometrics | 0.000 | 0.001 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| 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 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".