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Controlling Exsolution Dynamics in High-Entropy Oxides for Highly Active and Selective Acetylene Semi-Hydrogenation.

Hailing Yu^1,2, Caiqi Wang², Kevin M Siniard¹

¹Department of Chemistry, Institute for Advanced Materials and Manufacturing, University of Tennessee, Knoxville, Knoxville, Tennessee, USA.

Angewandte Chemie (International Ed. in English)

|May 15, 2026

Summary

Researchers engineered high-entropy oxides (HEOs) for catalysis. Tuning lattice and valence properties enabled controlled nanoparticle exsolution, creating a superior catalyst for acetylene semi-hydrogenation with enhanced activity and selectivity.

Keywords:

acetylene semi‐hydrogenation heterogeneous catalysis high entropy oxides lattice engineering metal exsolution

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Area of Science:

Materials Science
Catalysis
Nanotechnology

Background:

Exsolution-derived catalysts offer robust metal-support interactions for improved performance.
Precise control over exsolution dynamics in multicomponent oxides is a significant challenge.

Purpose of the Study:

To demonstrate rational tuning of exsolution behavior in high-entropy oxides (HEOs).
To create a highly active and selective catalyst for acetylene semi-hydrogenation via controlled exsolution.

Main Methods:

Incorporation of Li+ into a rock salt-structured HEO (LiNiMgCuZnCoO_x) for lattice and valence engineering.
Analysis of induced lattice distortion, oxygen vacancies, and Co site valence changes.
Studying the effect on nanoparticle exsolution dynamics and sequence.

Main Results:

Li+ incorporation modulated local charge redistribution, facilitating Cu nanoparticle exsolution.
Altered exsolution sequence from Cu0 > Ni0 > Co0 to Cu0 > Co0 > Ni0.
The resulting catalyst exhibited superior activity and ethylene selectivity in acetylene semi-hydrogenation.

Conclusions:

Coupled lattice and valence engineering in HEOs enables programmable exsolution.
This strategy provides a facile route to design high-performance catalysts.
Entropy-enabled engineering offers a promising approach for advanced catalytic applications.