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Entropy-Engineered Layered Double Hydroxide Derived High-Entropy Alloy Cathodes for Zinc-Air Batteries Under High
Nadar Allwyn1,2, Maria Antony Shalom1, Venkatraman Maithreyan1
1Electrochemical Power Sources Division, CSIR-CECRI, Karaikudi, Tamil Nadu, India.
Small (Weinheim an Der Bergstrasse, Germany)
|February 25, 2026
Summary
We developed a novel high-entropy alloy catalyst on nitrogen-doped carbon nanotubes for rechargeable zinc-air batteries (ZABs). This catalyst shows excellent bifunctional activity and durability, enabling high-performance ZAB applications.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Rechargeable zinc-air batteries (ZABs) require robust bifunctional electrocatalysts for oxygen reduction (ORR) and oxygen evolution (OER).
- High depths-of-discharge (DOD) performance is critical for practical ZAB applications.
- Developing efficient and stable catalysts remains a key challenge in advancing ZAB technology.
Purpose of the Study:
- To synthesize and characterize a novel high-entropy alloy (HEA) catalyst for bifunctional ORR and OER in ZABs.
- To investigate the structural and electrochemical properties of the HEA catalyst.
- To evaluate the performance and durability of ZABs utilizing the developed HEA catalyst.
Main Methods:
- Synthesis of a MnFeCoNiCu high-entropy alloy (HEA) anchored on nitrogen-doped carbon nanotubes (NCNTs) using a high-entropy layered double hydroxide precursor and dicyandiamide-assisted pyrolysis.
- Characterization of the HEA catalyst using structural and compositional analyses.
- Electrochemical testing of the HEA catalyst in a ZAB configuration, including ORR and OER performance, specific capacity, power density, and long-term cycling stability at high DOD.
Main Results:
- A single-phase face-centered cubic HEA (HEA 900) was successfully synthesized with uniform atomic-level metal dispersion and strong metal-carbon coupling.
- HEA 900 exhibited excellent bifunctional activity: OER overpotential of 475 mV at 10 mA/cm², ORR half-wave potential of 0.81 V, and a low ΔE of 0.89 V.
- The HEA-based ZAB demonstrated a high specific capacity (801 mAh/gZn), peak power density (186 mW/cm²), remarkable reversibility over 3325 cycles at high DOD, and robust performance in flexible gel-polymer ZABs.
Conclusions:
- The developed HEA catalyst exhibits superior bifunctional electrocatalytic activity and exceptional durability for rechargeable ZABs.
- The entropy-engineering strategy using HEA derived from layered double hydroxides offers a promising pathway for high-performance ZAB catalysts.
- This work highlights the potential of HEA catalysts for advanced energy storage applications, particularly in demanding ZAB systems.
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