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Ultrastable Bifunctional Electrocatalyst Based on High-Entropy Layered Hydroxide/Sulfide Heterostructure Enabled by

Zhonglu Hu¹, Fengqi Li¹, Hao Wu¹

¹National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093, P. R. China.

Langmuir : the ACS Journal of Surfaces and Colloids

|July 8, 2025

Summary

A new high-entropy catalyst efficiently produces hydrogen from seawater electrolysis. This durable material overcomes challenges in oxygen evolution reactions and material degradation, advancing sustainable energy.

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Area of Science:

Materials Science
Electrochemistry
Sustainable Energy

Background:

Electrocatalyst development is crucial for sustainable hydrogen production via water/seawater electrolysis.
Sluggish oxygen evolution reactions (OER) and material degradation in corrosive environments hinder efficiency.

Purpose of the Study:

To synthesize a novel high-entropy layered hydroxide/sulfide heterostructure composite (HELH/HEMS-6h) for efficient and durable electrocatalysis.
To investigate the role of cerium doping and heterostructure architecture in enhancing catalytic performance and stability.

Main Methods:

A two-step hydrothermal synthesis strategy was employed to create the HELH/HEMS-6h catalyst.
Characterization involved structural and electronic analyses to understand the catalyst's properties.
Electrochemical performance was evaluated for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in alkaline seawater media.

Main Results:

The optimized HELH/HEMS-6h catalyst demonstrated low overpotentials for OER (239 mV) and HER (71 mV) at 10 mA cm⁻².
Overall water splitting required only 1.55 V at 10 mA cm⁻² in alkaline seawater.
Cerium doping induced valence modulation and charge redistribution, enhancing active site exposure and chloride resistance.

Conclusions:

The HELH/HEMS-6h catalyst exhibits exceptional bifunctional activity and robust stability in seawater electrolysis.
Entropy-driven phase stabilization and interfacial electronic synergy contribute to the catalyst's durability.
This work presents a scalable approach for designing high-entropy electrocatalysts for practical hydrogen generation, promoting seawater electrolysis viability.