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Lanthanide Doping and Dual-Site Switching on Amorphous High-Entropy Metallene Oxides Boost Acidic Water Oxidation
Yinghao Li1, Yuntong Sun1, Mengshan Chen2
1School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang Drive, Singapore637459, Singapore.
Lanthanide-doped high-entropy oxides (HEOs) significantly boost oxygen evolution reaction (OER) efficiency. Optimized amorphous RuIrMnCoGd HEOs show remarkable stability and performance in acidic media and proton exchange membrane electrolyzers.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- High-entropy oxides (HEOs) are advanced electrocatalysts.
- Oxygen evolution reaction (OER) is crucial for energy conversion.
- Lanthanide doping is explored to enhance HEO performance.
Purpose of the Study:
- Investigate lanthanide doping effects on RuIr-based HEOs.
- Optimize HEO composition for superior OER activity and stability.
- Understand the fundamental mechanisms of enhanced catalysis.
Main Methods:
- Synthesis of amorphous RuIrMnCoGd high-entropy metallene oxides (a-Gd_HEMOs).
- Electrochemical testing in acidic media and proton exchange membrane electrolyzers.
- Operando characterizations and theoretical simulations (DFT).
Main Results:
- Optimized a-Gd_HEMOs achieved a low overpotential (211 mV) and long stability (700 h).
- Electrolyzer integration demonstrated high current density (3.0 A cm-2) and stable operation (300 h).
- Operando studies revealed electronic and coordination changes at active sites.
Conclusions:
- Lanthanide doping effectively enhances HEO electrocatalytic properties for OER.
- The optimized HEOs exhibit excellent performance and durability in acidic conditions.
- Synergistic effects and dynamic active site switching contribute to robust oxygen generation.
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