Exploring fuel cell cathode materials using ab initio high throughput calculations and validation using carbon...

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• The oxygen reduction reaction (ORR) is crucial for fuel cell performance.
• Developing efficient and stable ORR catalysts is essential for advancing clean energy technologies.

Purpose of the Study:

• To screen a wide range of M elements and Pt3M alloys for ORR activity and stability.
• To validate computational predictions with experimental data.
• To assess the reliability of DFT descriptors for catalyst design.

Main Methods:

• Combined density functional theory (DFT) calculations and experimental screening.
• Synthesis and characterization of carbon-supported alloy nanoparticles.
• Electrochemical measurements in membrane electrode assembly (MEA) environments.

Main Results:

• DFT calculations predicted the ORR activity and stability of various Pt3M alloys.
• Experimental validation confirmed correlations between computed descriptors (d-band center, O adsorption energy) and ORR performance.
• Calculated segregation energies correlated with base metal leaching, and O adsorption energies correlated with ORR activity.

Conclusions:

• The combined DFT and experimental approach effectively screens potential ORR catalysts.
• Surface segregation of base metals is a key factor influencing catalyst stability.
• Computed O adsorption energy is a reliable descriptor for predicting ORR activity in Pt3M alloys.