journal article·2025-08

Deciphering the Synergy of Multiple Vacancies in High‐Entropy Layered Double Hydroxides for Efficient Oxygen Electrocatalysis

Yiyue Zhai, Xiangrong Ren, Tao Gan, Liaona She, Qingjun Guo, Na Yang, Bolun Wang, Yao Yao, Shengzhong (Frank) Liu

Advanced Energy Materials· Volume 15· Issue 30
Publisher page

Abstract

Abstract Layered double hydroxides (LDHs) hold the promise of designing efficient and long‐lived electrocatalysts for alkaline oxygen evolution reaction (OER), yet control of their activity and durability at ampere‐scale current densities remains a challenge. Here, a high‐entropy LDH anode integrating multiple metal and oxygen vacancies is reported that achieves superior and robust OER under industrial conditions. The molar ratio of Ni:Cr:Co:Zn:Fe in high‐entropy LDHs engineers the electronic structure via the cocktail effect, yielding more high‐valent metal ions that promote the electrochemical restructuring. Using various operando characterizations, the generation of γ‐NiOOH active‐phase on a high‐entropy LDH surface is identified, triggering the oxygen‐vacancy‐site mechanism (OVSM). Importantly, a volcano relationship is found between intrinsic OER activity (overpotential value) and the local coordination structure of Ni active centers (matching with the ΔG*OH). The integration of multiple metal and oxygen vacancies significantly optimizes the adsorption‐free energy of oxygen‐containing intermediates that are anchored at Ni active sites, boosting the OVSM. Accordingly, the developed Ni0.15Cr0.15Co0.4Zn0.1Fe0.2‐LDH@NF achieves 1 A·cm−2 at 1.81 V and enables stable operation over 300 h in anion exchange membrane water electrolyzer. These findings elucidate the synergistic effects of multiple vacancies in high‐entropy LDH electrocatalysts and enlighten the vacancy engineering for designing high‐efficiency OER catalysts.
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Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Advanced battery technologies research · Fuel Cells and Related Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Civil & Architecture Engineering Xi'an Technological University Xi'an 710021 P. R. China

Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science and Engineering Shaanxi Normal University Xi'an 710119 P. R. China

Institute of Science and Technology for New Energy Xi'an Technological University Xi'an 710021 P. R. China

Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 P. R. China

School of Materials and Energy University of Electronic Science and Technology of China Chengdu 611731 P. R. China

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry International Center of Future Science Jilin University Changchun 130012 P. R. China

Key Laboratory of Photoelectric Conversion and Utilization of Solar Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian Liaoning 116023 P. R. China

Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 P. R. China

CNNP Optoelectronics Technology 2828 Canghai Road, Lingang Shanghai 201308 P. R. China

Funding

Higher Education Discipline Innovation Project · National Natural Science Foundation of China

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