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Building Topological-Disordered High-Entropy Amorphous Oxides for Adaptive Compensation During Alternating CO2 Redox

Yuchun Liu1, Tianqi Liu1, Zhixin Sun1

  • 1Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.

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High-entropy amorphous oxides with topological disorder engineering prevent material fatigue in electrochemical applications. This approach enhances durability and performance by enabling self-adaptive compensation under stress.

Keywords:
Adaptive compensationFatigue‐resistant materialsHigh entropy amorphous oxidesLi‐CO2 batteryTopological disorder

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Nanotechnology

Background:

  • Material fatigue from structural changes degrades electrochemical device performance.
  • Preserving active-site durability is a key challenge in electrochemical systems.
  • Topological disorder engineering offers a pathway to enhance structural stability and reaction kinetics.

Purpose of the Study:

  • To introduce high-entropy amorphous oxides (HEAOs) as a model system for topological disorder engineering.
  • To investigate the self-adaptive mechanisms in HEAOs for mitigating electrochemical fatigue.
  • To demonstrate the effectiveness of HEAOs in enhancing electrochemical performance and durability.

Main Methods:

  • Synthesis of high-entropy amorphous oxides (HEAOs).
  • Characterization of the dynamic metal-oxygen coordination network and electronic interactions (d-d electron transfer, d-p orbital coupling).
  • Electrochemical testing in Li-CO2 batteries, including cycling performance and energy efficiency measurements.

Main Results:

  • HEAOs exhibit intrinsic self-adaptive topological disorder with exceptional structural relaxation.
  • Flexible M-O-M linkages and multicomponent integration induce electronic interactions for charge redistribution.
  • In Li-CO2 batteries, HEAOs achieved an ultra-high discharge voltage (3.14 V) and maintained ~90% energy efficiency over long-term cycling.

Conclusions:

  • Topological disorder engineering in HEAOs provides long-range integrity and suppresses electrochemical fatigue.
  • Self-adaptive compensation in HEAOs arises from responsive topologically disordered metal-oxygen polyhedra, mitigating strain accumulation.
  • Long-range topological adaptability is a crucial design principle for fatigue-resistant electrochemical materials.