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Intermetallic Pd3Pb nanocubes with high selectivity for the 4-electron oxygen reduction reaction pathway
Jocelyn T L Gamler1, Kihyun Shin2, Hannah M Ashberry1
1Department of Chemistry, Indiana University - Bloomington, 800 E. Kirkwood Ave., Bloomington, IN 47405, USA. sskrabal@indiana.edu.
Nanoscale
|January 15, 2020
Summary
Palladium-lead (Pd-Pb) intermetallic nanocubes efficiently catalyze the oxygen reduction reaction (ORR) in fuel cells. This new synthesis method yields superior electrocatalysts with enhanced activity and selectivity for the desired 4-electron pathway.
Area of Science:
- Nanomaterials Science
- Electrochemistry
- Catalysis
Background:
- Platinum-based catalysts are standard for fuel cell reactions but are expensive.
- Palladium-based intermetallic nanomaterials show promise as alternatives for oxygen reduction reactions (ORR) in alkaline media.
- Synthesis of shape-controlled palladium-based intermetallic nanoparticles remains a significant challenge.
Purpose of the Study:
- To develop a low-temperature synthesis method for intermetallic Palladium-3-Lead (Pd3Pb) nanocubes.
- To evaluate the electrocatalytic properties of Pd3Pb nanocubes for the ORR.
- To investigate the mechanism behind the enhanced catalytic activity using density functional theory (DFT) calculations.
Main Methods:
- Low-temperature synthesis of intermetallic Pd3Pb nanocubes.
- Electrocatalytic evaluation of Pd3Pb nanocubes for ORR in alkaline media.
- Tafel analysis to determine the reaction pathway selectivity.
- Density functional theory (DFT) calculations to understand adsorption mechanisms.
Main Results:
- The synthesized intermetallic Pd3Pb nanocubes demonstrated superior ORR electrocatalytic activity compared to commercial Pd/C and Pd nanocube references.
- A mass activity of 154 mA mgPd−1 was achieved, representing a 130% increase over Pd/C and a 230% increase over Pd nanocubes.
- Tafel analysis indicated high selectivity for the 4-electron ORR pathway, with minimal hydrogen peroxide (HO2−) formation.
- DFT calculations suggested that weakened hydroxyl (OH*) adsorption on Pd3Pb contributes to reduced overpotential and increased activity.
Conclusions:
- Intermetallic Pd3Pb nanocubes are highly efficient electrocatalysts for the 4-electron ORR pathway.
- The developed low-temperature synthesis offers a viable route to shape-controlled intermetallic nanocatalysts.
- These findings encourage further research into other shape-controlled intermetallic compounds for advanced fuel cell applications.
