Axial engineering of bilayer single-atom catalysts for enhanced bifunctional oxygen electrocatalysis
Xinge Wu1, Wenzhu Tan1, Zhaoying Yang1
1College of Sciences, Northeastern University, Shenyang 110819, China.
Physical Chemistry Chemical Physics : PCCP
|September 5, 2025
Summary
Engineered bilayer single-atom catalysts (SACs) with axial ligands show enhanced stability and bifunctional activity for oxygen reduction and evolution reactions. This design overcomes limitations of monolayer SACs, paving the way for efficient electrocatalysts.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Single-atom catalysts (SACs) are crucial for electrocatalysis, but monolayer SACs with single axial ligands lack stability.
- Axial ligand engineering is a key strategy to improve SAC performance.
Purpose of the Study:
- To design and screen novel bilayer SACs (BSACs) with enhanced stability and bifunctional oxygen reduction (ORR) and oxygen evolution (OER) activity.
- To investigate the role of axial non-metallic atoms in stabilizing BSACs and optimizing catalytic performance.
Main Methods:
- High-throughput density functional theory (DFT) screening of 60 BSAC candidates with varying metal (Sc-Zn) and axial ligands (C, N, O, P, S, Se).
- Analysis of electronic structures to understand the mechanism of enhanced catalytic activity.
Main Results:
- Identified FeN4-P-MnN4 (P-FeMn) and FeN4-C-MnN4 (C-FeMn) as highly active bifunctional electrocatalysts for ORR/OER.
- Achieved low overpotentials for ORR (0.27-0.37 V) and OER (0.31-0.42 V).
- Axial P/C atoms induced spin transitions and weakened metal-oxygen orbital hybridization, enhancing activity.
Conclusions:
- Bilayer SACs with axial ligand engineering offer superior stability and bifunctional catalytic activity compared to monolayer SACs.
- The designed BSACs provide a promising platform for developing efficient and stable oxygen electrocatalysts.
- This study offers new strategies for designing advanced single-atom catalysts for energy applications.
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