High-entropy engineering with regulated defect structure and electron interaction tuning active sites for...

Area of Science:

• Materials Science
• Electrochemistry
• Nanotechnology

Background:

• High-entropy alloy nanoparticles (HEANs) offer tunable defect structures and electron interactions for catalyst development.
• The microstructure-activity relationship of HEANs in multifunctional electrocatalysis remains underexplored.

Purpose of the Study:

• To investigate the mechanism of trifunctional electrocatalysis (oxygen reduction, oxygen evolution, hydrogen evolution) using HEANs distributed on multi-walled carbon nanotubes (HEAN/CNT).
• To establish the microstructure-activity relationship for HEANs as multifunctional electrocatalysts.

Main Methods:

• Preparation of HEAN/CNT using Joule heating.
• In situ monitoring and theoretical calculations (density functional theory) to study electrocatalytic mechanisms.
• Investigation of defect structure and electron interaction characteristics.

Main Results:

• HEAN/CNT exhibits exceptional stability in zinc-air batteries (0.8V for 220h) and water electrolysis (undiminished after 20h).
• Detailed characterization of intrinsic defect structure and electron interaction in HEAN/CNT.
• Identification of the trifunctional electrocatalytic mechanism through in situ monitoring and theoretical validation.

Conclusions:

• The study provides insights into the microstructure-activity relationship of HEANs for trifunctional electrocatalysis.
• Findings offer a pathway for designing cost-effective, multifunctional high-entropy electrocatalysts.