High-Entropy Alloy Aerogels with High-Density Solid–Solid Heterointerfaces for Alkaline Hydrogen Evolution

Abstract

Constructing high-entropy alloy (HEA)-based solid–solid heterointerfaces offers a powerful route to creating catalytic materials with high structural complexity, particularly through the formation of grain-boundary-rich architectures. Such internal heterointerfaces provide diverse local atomic configurations that can enable interfacial synergy, circumvent scaling relations, and optimize multistep reaction pathways. However, the realization of HEA-based solid–solid heterostructures at the nanoscale remains challenging due to the stringent synthesis conditions and intrinsic atomic disorder of HEAs. Here, we report an epitaxial assembly strategy that drives the self-assembly of colloidal HEA nanoparticles into a self-supported three-dimensional aerogel, in which the particles are interconnected by epitaxially grown metal domains, forming extended heterostructures with abundant grain boundaries. Using alkaline hydrogen evolution as a model reaction, we show that the resulting HEA|Pt heterostructured aerogel exhibits significantly enhanced catalytic activity compared to isolated HEA nanoparticles, delivering overpotentials of 51 mV and 109 mV at 100 mA cm–2, respectively. Combined kinetic analyses and density functional theory calculations reveal that hydrogen coupling on the HEA surface is inhibited by strongly adsorbed hydroxyl species, whereas the HEA|Pt heterointerfaces lower the water dissociation barrier and enable interfacial hydrogen spillover from HEA to Pt, thereby facilitating efficient hydrogen recombination. This work establishes a general nanoscale strategy for engineering grain-boundary-dominated HEA heterostructures and opens new opportunities for assembling complex colloidal architectures with emergent interfacial functionalities.

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Cite

BibTeX RIS

BibTeX

@article{wang2026highentropy,
  title = {{High-Entropy Alloy Aerogels with High-Density Solid–Solid Heterointerfaces for Alkaline Hydrogen Evolution}},
  author = {Lingwei Wang and Shiyu Zhen and Varatharaja Nallathambi and Cui Wang and Xiaoyue Shi and Ning Lu and René Hübner and Alexander Eychmüller and Sven Reichenberger and Baptiste Gault and Liang Zhang and Bin Cai},
  journal = {Journal of the American Chemical Society},
  year = {2026},
  month = may,
  doi = {10.1021/jacs.6c02377},
  url = {https://hal.science/hal-05762326v1},
  note = {CC BY 4.0},
}

RIS

TY  - JOUR
TI  - High-Entropy Alloy Aerogels with High-Density Solid–Solid Heterointerfaces for Alkaline Hydrogen Evolution
AU  - Lingwei Wang
AU  - Shiyu Zhen
AU  - Varatharaja Nallathambi
AU  - Cui Wang
AU  - Xiaoyue Shi
AU  - Ning Lu
AU  - René Hübner
AU  - Alexander Eychmüller
AU  - Sven Reichenberger
AU  - Baptiste Gault
AU  - Liang Zhang
AU  - Bin Cai
PY  - 2026
DA  - 2026/05/28
JO  - Journal of the American Chemical Society
DO  - 10.1021/jacs.6c02377
UR  - https://hal.science/hal-05762326v1
AB  - Constructing high-entropy alloy (HEA)-based solid–solid heterointerfaces offers a powerful route to creating catalytic materials with high structural complexity, particularly through the formation of grain-boundary-rich architectures. Such internal heterointerfaces provide diverse local atomic configurations that can enable interfacial synergy, circumvent scaling relations, and optimize multistep reaction pathways. However, the realization of HEA-based solid–solid heterostructures at the nanoscale remains challenging due to the stringent synthesis conditions and intrinsic atomic disorder of HEAs. Here, we report an epitaxial assembly strategy that drives the self-assembly of colloidal HEA nanoparticles into a self-supported three-dimensional aerogel, in which the particles are interconnected by epitaxially grown metal domains, forming extended heterostructures with abundant grain boundaries. Using alkaline hydrogen evolution as a model reaction, we show that the resulting HEA|Pt heterostructured aerogel exhibits significantly enhanced catalytic activity compared to isolated HEA nanoparticles, delivering overpotentials of 51 mV and 109 mV at 100 mA cm–2, respectively. Combined kinetic analyses and density functional theory calculations reveal that hydrogen coupling on the HEA surface is inhibited by strongly adsorbed hydroxyl species, whereas the HEA|Pt heterointerfaces lower the water dissociation barrier and enable interfacial hydrogen spillover from HEA to Pt, thereby facilitating efficient hydrogen recombination. This work establishes a general nanoscale strategy for engineering grain-boundary-dominated HEA heterostructures and opens new opportunities for assembling complex colloidal architectures with emergent interfacial functionalities.
SN  - 0002-7863
SN  - 1520-5126
ER  -

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