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Updated: May 9, 2026
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Published on: December 6, 2021
Ultrafine Nanoporous Ordered High-Entropy Intermetallics with Isolated Multisites toward Electrocatalytic Aldehyde
Jilong Li1, Zhen Wang1, Linghu Meng1
1College of Materials Science and Engineering, State Key Laboratory of Advanced Design and Manufacturing Technology for Vehicle, Hunan University, Changsha, Hunan 410082, China.
None:
Developing high-efficiency alloy catalysts toward electrocatalytic hydrogenation is crucial for large-scale sustainable chemical transformations, but traditional single-principal-element alloys usually suffer from insufficient activity and stability due to randomly dispersed active sites and limited electron-donating ability. Here, we report a Zn-assisted electrochemical phase transformation (Zn-EPT) strategy to synthesize ultrafine nanoporous (∼2 nm) high-entropy intermetallics (np-HEIs) featuring spatially isolated multisites under mild conditions, utilizing the low melting point and mixing enthalpy of Zn as a sacrificial element to incorporate disparate metals into a nanoporous body-centered framework. Among all candidates, the nanoporous (Pd0.25Cu0.25Ag0.25Ir0.25)Zn (np-PCAIZ) achieves exceptional electrocatalytic furfural hydrogenation performance with 93.8% conversion, 92.4% FE, and 100% selectivity at -0.2 V vs RHE and demonstrates outstanding stability over 120 h at 100 mA cm-2 in a membrane electrode assembly for gram-scale production of furfuryl alcohol. Theoretical calculations combined with experimental results reveal that the ordered high-entropy structure and isolated multisites of np-PCAIZ optimize the η2-(C, O)-aldehyde adsorption configuration for C═O bond activation and facilitate a highly interconnected two-coordinated hydrogen-bonded network for directional H* transfer and suppressing the competitive hydrogen evolution reaction (HER). The presented Zn-EPT strategy for synthesizing ultrafine np-HEIs offers a general blueprint for designing high-efficiency electrocatalysts for electrocatalytic hydrogenation and other related applications.
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