biostudies-literatureZou XMOST | National Natural Science Foundation of China (NSFC)| Major Science and Technology Projects in Yunnan Province ()云南省科学技术厅 | Major Science and Technology Projects in Yunnan ProvinceMOST | National Natural Science Foundation of Chinae2313239121https://www.ebi.ac.uk/biostudies/studies/S-EPMC10990096biostudies-literatureUnknown121(13)High-entropy alloy nanoparticles (HEANs) possessing regulated defect structure and electron interaction exhibit a guideline for constructing multifunctional catalysts. However, the microstructure-activity relationship between active sites of HEANs for multifunctional electrocatalysts is rarely reported. In this work, HEANs distributed on multi-walled carbon nanotubes (HEAN/CNT) are prepared by Joule heating as an example to explain the mechanism of trifunctional electrocatalysis for oxygen reduction, oxygen evolution, and hydrogen evolution reaction. HEAN/CNT excels with unmatched stability, maintaining a 0.8V voltage window for 220 h in zinc-air batteries. Even after 20 h of water electrolysis, its performance remains undiminished, highlighting exceptional endurance and reliability. MoreoProceedings of the National Academy of Sciences of the United States of AmericaHigh-entropy engineering with regulated defect structure and electron interaction tuning active sites for trifunctional electrocatalysis.PMC10990096202302AB080019-352064049Sheng XMei ZJing QWang LZou XSun MRen FYang YHe TGuo HXie JZhang CKong YfalseHigh-entropy engineering with regulated defect structure and electron interaction tuning active sites for trifunctional electrocatalysis.High-entropy alloy nanoparticles (HEANs) possessing regulated defect structure and electron interaction exhibit a guideline for constructing multifunctional catalysts. However, the microstructure-activity relationship between active sites of HEANs for multifunctional electrocatalysts is rarely reported. In this work, HEANs distributed on multi-walled carbon nanotubes (HEAN/CNT) are prepared by Joule heating as an example to explain the mechanism of trifunctional electrocatalysis for oxygen reduction, oxygen evolution, and hydrogen evolution reaction. HEAN/CNT excels with unmatched stability, maintaining a 0.8V voltage window for 220 h in zinc-air batteries. Even after 20 h of water electrolysis, its performance remains undiminished, highlighting exceptional endurance and reliability. Moreo2024-01-01T00:00:00Z2024 Mar2025-04-20T00:45:13.318Z2025-04-20T00:45:13.318ZS-EPMC109900963849871010.1073/pnas.2313239121