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Tuning intermediate adsorption in structurally ordered substituted PdCu3 intermetallic nanoparticles for enhanced
Rajkumar Jana1, Ayan Datta, Sudip Malik
1School of Chemical Sciences, Indian Association for the Cultivation of Science, Kolkata-700032, India. spad@iacs.res.in.
Chemical Communications (Cambridge, England)
|May 6, 2021
Summary
Cobalt and Nickel-substituted palladium-copper intermetallic nanoparticles significantly boost ethanol electrooxidation (EOR) activity and durability. This enhancement stems from improved radical generation and electronic structure modifications, as revealed by first-principle calculations.
Area of Science:
- Electrochemistry
- Materials Science
- Nanotechnology
Background:
- Ethanol electrooxidation (EOR) is crucial for fuel cells.
- Developing efficient and durable electrocatalysts is essential for EOR.
- Palladium-copper (PdCu) intermetallic nanoparticles show promise but require further optimization.
Purpose of the Study:
- To investigate the effect of Cobalt (Co) and Nickel (Ni) substitution on PdCu3 nanoparticles for enhanced EOR.
- To understand the underlying mechanisms responsible for improved electrocatalytic activity and durability.
Main Methods:
- Synthesis of structurally ordered intermetallic PdCu3 nanoparticles with Co and Ni substitution at low temperatures.
- Electrochemical testing to evaluate ethanol electrooxidation activity and durability.
- First-principle calculations to elucidate the electronic structure and reaction mechanisms.
Main Results:
- Co and Ni-substituted PdCu3 nanoparticles exhibited significantly enhanced EOR activity and improved durability compared to unsubstituted counterparts.
- First-principle calculations indicated that substitution promotes the proximity of OH and CH3CO radicals.
- Calculations also revealed a shift in the d-band center towards the Fermi level, contributing to boosted EOR efficiency.
Conclusions:
- Low-temperature synthesis of Co and Ni-substituted intermetallic PdCu3 nanoparticles offers a promising strategy for advanced EOR electrocatalysts.
- The enhanced performance is attributed to synergistic effects including optimized radical generation and electronic structure modulation.
- This study provides fundamental insights into catalyst design for efficient ethanol electrooxidation.
