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Regulating the Electronic Structure via Multi-Transition Metals in Nanoporous High-Entropy Perovskites for Boosted
Min Xue1, Wenchao Zhang1, Yiwei Ding1
1Shandong Provincial Key Laboratory of Processing and Testing Technology of Glass & Functional Ceramics, School of Materials Science and Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan, China.
High-entropy perovskite oxides (HEPOs) show promise for electrocatalysis. Nanoporous HEPOs were synthesized and demonstrated exceptional activity and stability for the alkaline hydrogen evolution reaction (HER), outperforming platinum/carbon.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- High-entropy perovskite oxides (HEPOs) offer vast compositional flexibility for designing advanced electrocatalysts.
- The hydrogen evolution reaction (HER) is crucial for clean energy technologies, requiring efficient and stable catalysts.
Purpose of the Study:
- To synthesize novel nanoporous La-based HEPOs for alkaline HER.
- To investigate the structure-property relationships governing the electrocatalytic performance of these HEPOs.
- To evaluate their potential in overall water-splitting systems.
Main Methods:
- Synthesis of La-based HEPOs via dealloying and annealing.
- Electrocatalytic testing for alkaline HER, including overpotential and Tafel slope measurements.
- Structural characterization (e.g., X-ray diffraction), in situ Raman spectroscopy, and density functional theory (DFT) calculations.
Main Results:
- Successfully synthesized single-phase cubic nanoporous HEPOs.
- L5M-0Cr exhibited superior alkaline HER activity (low overpotential of ~50.6 mV at -10 mA cm⁻², Tafel slope of ~60.1 mV dec⁻¹), surpassing Pt/C at high current densities.
- Demonstrated excellent stability (>120 h) and promising performance in overall water splitting.
Conclusions:
- High-entropy design in perovskites synergistically optimizes structural, electronic, and catalytic properties.
- Lattice distortion and charge redistribution in HEPOs enhance electronic structure and HER activity.
- This strategy provides a new avenue for developing efficient electrocatalysts for energy conversion.
