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Coordination Engineering Induced d-Band Center Shift on Single-Atom Fe Electrocatalysts for Enhanced Oxygen Reduction
Huimin Liu1, Chen Wang1, Chang Liu1
1School of Chemical Engineering, University of Science and Technology Liaoning, 185 Qianshan Zhong Road, Anshan 114051, P. R. China.
ACS Applied Materials & Interfaces
|June 6, 2023
Summary
This study introduces a novel iron single-atom catalyst (Fe-SNC) with unique N,S coordination and hydroxyl groups, demonstrating enhanced oxygen reduction reaction (ORR) activity and stability for zinc-air batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Single-atom catalysts (SACs) performance is highly dependent on the local microenvironment.
- Understanding the precise regulation of catalytic activity by coordination environments remains a challenge.
Purpose of the Study:
- To synthesize and characterize a novel single-atom catalyst with tailored coordination for improved oxygen reduction reaction (ORR).
- To investigate the influence of sulfur and hydroxyl coordination on the catalytic activity and stability of iron-based SACs.
- To evaluate the performance of the developed catalyst in rechargeable zinc-air batteries.
Main Methods:
- Synthesis of a hierarchically porous carbon material embedded with a single Fe active center (Fe-SNC) featuring asymmetric N,S coordination and an axial hydroxyl group.
- Electrochemical characterization of the Fe-SNC catalyst for ORR activity and stability.
- Assembly and testing of a rechargeable Zn-air battery utilizing the Fe-SNC catalyst.
Main Results:
- The prepared Fe-SNC catalyst exhibited superior ORR activity and stability compared to commercial Pt/C and other reported SACs.
- Introduction of S atoms facilitated porous structure formation and optimized oxygen intermediate adsorption/desorption.
- Axial OH groups reduced ORR intermediate bonding strength and optimized the Fe d-band center.
Conclusions:
- The Fe-SNC catalyst demonstrates significant potential for efficient ORR catalysis.
- Tailoring the electrocatalyst microenvironment through precise coordination engineering is crucial for enhancing catalytic performance.
- This work provides insights for the multiscale design of electrocatalysts for energy applications.
Keywords:
Zn−air batteriesmicroenvironment modulationoxygen reduction reactionpenta-coordinated configurationsingle-atom catalystsMore Related Videos
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