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In Situ Raman Spectroscopy Correlates *OOH Intermediates with Oxygen Reduction Activity on Pt-Based Nanocatalysts
Lie Zou1, Xiao-Yan Huang2, Yi Zhang2
1State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian116024, China.
ACS Applied Materials & Interfaces
|August 13, 2026
Summary
Platinum-nickel (PtNi) alloys enhance oxygen reduction reaction (ORR) electrocatalysis by optimizing the key *OOH intermediate. This study reveals molecular insights into ORR activity on Pt-based catalysts using in situ Raman spectroscopy.
Area of Science:
- Electrochemistry
- Materials Science
- Surface Science
Background:
- Understanding the oxygen reduction reaction (ORR) on platinum-based catalysts is crucial for designing efficient electrocatalysts.
- The molecular mechanisms governing ORR activity on alloyed platinum catalysts remain incompletely understood.
Purpose of the Study:
- To investigate the ORR pathway on Pt-based alloy nanocatalysts with varying transition metals.
- To elucidate how surface oxygenated intermediates influence ORR activity.
- To establish a correlation between intermediate adsorption and catalytic performance.
Main Methods:
- Electrochemical measurements to assess ORR activity.
- In situ shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) to probe reaction intermediates.
- Isotopic labeling to confirm intermediate identification.
Main Results:
- PtNi catalysts demonstrated superior ORR activity compared to PtFe, PtCo, and commercial Pt/C.
- In situ Raman spectroscopy identified *OOH as a key intermediate, with its vibrational frequency correlating to ORR activity.
- Ni alloying was found to weaken Pt-O interactions and optimize *OOH adsorption.
Conclusions:
- The study provides molecular-level understanding of ORR activity enhancement in Pt-based alloys.
- Ni alloying optimizes the electronic structure of Pt, promoting ORR kinetics.
- An effective spectroscopic platform for probing ORR intermediates on realistic electrocatalyst surfaces was established.
Keywords:
Pt-based alloy catalystsSHINERSin situ Raman spectroscopyoxygen reduction reactionreaction intermediatesMore Related Videos
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