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Pd 4d Orbital Overlapping Modulation on Au@Pd Nanowires for Efficient H2O2 Production
Zhiping Deng1, Amir Hassan Bagherzadeh Mostaghimi2, Mingxing Gong3
1Department of Chemical and Materials Engineering, University of Alberta, 9211-116 Street NW., Edmonton, Alberta T6G 1H9, Canada.
Journal of the American Chemical Society
|January 17, 2024
Summary
The study found that Pd4 clusters, not Pd3, are optimal for the 2e- oxygen reduction reaction (ORR), achieving high H2O2 selectivity and activity. This discovery advances electrocatalyst design for efficient ORR performance.
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- Designing palladium (Pd)-based electrocatalysts for the 2-electron (2e-) oxygen reduction reaction (ORR) is critical.
- Optimal balance between activity and selectivity in 2e- ORR electrocatalysts remains a challenge.
Purpose of the Study:
- Investigate the influence of Pd 4d orbital overlap on 2e- ORR performance using Au@Pd core@shell structures.
- Determine the optimal Pd cluster size for enhanced H2O2 selectivity and activity.
Main Methods:
- Synthesis of Au@Pd core@shell structures.
- Density Functional Theory (DFT) calculations.
- Electrochemical evaluation of catalytic performance in acidic electrolyte.
Main Results:
- DFT predicted Pd clusters with n ≤ 3 favor H2O2 selectivity for 2e- ORR.
- Experimental results identified Au@Pd nanowires with Pd4 as the optimal structure for 2e- ORR.
- Achieved high mass activity (7.05 A mg⁻¹) and H2O2 selectivity (nearly 95%) with Pd4.
Conclusions:
- Pd4 clusters represent the upper size threshold for ideal 2e- ORR, contrary to previous predictions.
- Oxygen coverage during ORR on Pd4 leads to electron redistribution and weakened *OOH binding, enhancing activity.
- The optimal Pd4 structure exhibits a low overpotential (0.06 V) in acidic media.
