Chlorine Axial Coordination Activated Lanthanum Single Atoms for Efficient Oxygen Electroreduction with Maximum...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Designing effective electrocatalysts for rare-earth (RE) elements remains challenging.
• Activating RE elements for intrinsic electrocatalytic reactivity requires rational ligand field design.

Purpose of the Study:

• To construct La single atoms (La-Cl SAs/NHPC) with high oxygen reduction reaction (ORR) activity.
• To explore the potential of RE-based catalysts in energy storage applications like zinc-air batteries (ZABs).

Main Methods:

• Utilized axial coordination strategies and nanostructure design to synthesize La-Cl SAs/NHPC.
• Investigated the catalyst's performance in alkaline media for ORR and in aqueous/flexible ZABs.
• Employed theoretical calculations to understand the electronic structure modulation and reaction mechanisms.

Main Results:

• Achieved a high half-wave potential of 0.91 V for ORR with La-Cl SAs/NHPC.
• Demonstrated significant robustness in alkaline media and high power densities (260.7 mW cm⁻²) in ZABs.
• Theoretical calculations confirmed Cl coordination enhances La site electroactivity and optimizes intermediate adsorption.

Conclusions:

• The La-Cl SAs/NHPC catalyst exhibits excellent ORR activity and stability, making it a promising RE-based electrocatalyst.
• The developed preparation strategy, focusing on electronic structure modulation via nonplanar coordination, is applicable to other RE elements.
• This work provides valuable insights for designing efficient RE-single-atom electrocatalysts for energy conversion applications.