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High-Entropy Metal–Organic Framework-Based Armor Catalysts for Electrocatalytic Water Splitting: A Comprehensive Review
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DOI：10.1002/cctc.70900.png)
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Abstract
En 中文
Electrocatalytic water splitting is pivotal for sustainable hydrogen production but is constrained by the sluggish kinetics of the oxygen evolution reaction (OER) and the inherent activity-stability trade-off. To address these limitations, high-entropy metal–organic framework (HE-MOF) based armor catalysts have emerged as a promising platform. This innovative design ingeniously combines the thermodynamic stabilization and synergistic effects of high-entropy alloys with the structural tunability of MOFs. By constructing a robust protective “armor” around the active high-entropy core, these catalysts successfully decouple intrinsic catalytic activity from long-term durability, effectively mitigating key degradation pathways such as active-site leaching and agglomeration. This comprehensive review systematically elucidates the fundamental principles of high-entropy and core–shell armor architectures. We critically analyze advanced synthesis strategies and detail how electronic modulation and strain engineering optimize reaction intermediate adsorption. Their superior performance in pH-universal hydrogen evolution, oxygen evolution, and overall water splitting is thoroughly discussed. Finally, current challenges and future perspectives toward AI-guided design and scalable integration are outlined, providing a roadmap for next-generation electrocatalyst development.
Keywords:
core–shell armor catalysts
electrocatalytic water splitting
high-entropy metal–organic frameworks
structure-activity relationship
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