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Updated: May 31, 2025
Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
Quantifying Asymmetric Coordination to Correlate with Oxygen Reduction Activity in Fe-Based Single-Atom Catalysts
Yanhui Cao1, Yuan Liu1, Xuerong Zheng1,2
1School of Materials Science and Engineering, State Key Laboratory of Precious Metal Functional Materials, Tianjin Key Laboratory of Composite and Functional Materials, Key Laboratory of Advanced Ceramics and Machining Technology (Ministry of Education), Tianjin University, Tianjin, 300072, P. R. China.
Researchers developed an "asymmetry degree" to quantify catalyst configurations, optimizing single-atom catalysts (SACs) for the oxygen reduction reaction (ORR). Moderate asymmetry enhances catalytic activity by tuning electronic properties.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Single-atom catalysts (SACs) offer high efficiency for the oxygen reduction reaction (ORR).
- Tuning coordination configuration and electronic effects is crucial for optimizing SAC intrinsic activity.
- Current design strategies for SACs lack a clear relationship between coordination asymmetry and catalytic performance.
Purpose of the Study:
- To introduce a quantitative measure, "asymmetry degree," for coordination configurations in SACs.
- To establish a theoretical framework linking asymmetry degree to ORR activity in Fe-based SACs.
- To provide rational guidance for designing high-performance SACs with asymmetric configurations.
Main Methods:
- Computational modeling of Fe-based SACs with varying non-metal dopants (B, P, S, Se, Te).
- Theoretical framework elucidating the volcano relationship between asymmetry degree and ORR activity.
- Experimental validation of predicted ORR activity using the asymmetry degree concept.
Main Results:
- A quantitative "asymmetry degree" was proposed to characterize coordination configurations.
- A volcano relationship between asymmetry degree and ORR activity was established, aligning with the Sabatier principle.
- Moderate asymmetry in Fe-based SACs was found to optimize intrinsic ORR activity.
Conclusions:
- Breaking the square-planar symmetry of FeN4 enhances ORR activity by optimizing Fe 3d-orbital electronic populations.
- A moderate asymmetry degree is optimal for intrinsic ORR activity in SACs.
- This work provides fundamental insights for designing high-performance asymmetric SACs.
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