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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
Geminal Cl-Bridged Dual-Fe-Atom Catalyst for Efficient and Stable Oxygen Reduction Reaction
Junjie Cui1, Wenyao Zhang1, Yangrui Hou1
1Key Laboratory for Soft Chemistry and Functional Materials of Ministry Education, School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
Researchers developed a stable dual-iron atom catalyst by understanding iron-nitrogen-carbon catalyst degradation. This new catalyst shows remarkable durability for the oxygen reduction reaction (ORR) in batteries.
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- Atomically dispersed iron-nitrogen-carbon (Fe-N-C) catalysts are promising for the oxygen reduction reaction (ORR).
- Structural instability and iron demetallization limit the practical application of Fe-N-C catalysts.
- Understanding the degradation mechanism is crucial for designing robust catalysts.
Purpose of the Study:
- To elucidate the mechanism of electrochemical degradation in Fe-N-C catalysts during ORR.
- To design and synthesize a novel dual-Fe-atom catalyst with enhanced structural stability.
- To investigate the role of catalyst structure in ORR performance and durability.
Main Methods:
- Mechanistic studies to identify the cause of Fe demetallization.
- Synthesis of a dual-Fe-atom catalyst with a N3-Fe-Cl-Fe-N3 structure.
- Theoretical calculations and experimental validation (electrochemical testing, durability cycling, zinc-air battery performance).
Main Results:
- Electrochemical degradation of Fe-N-C catalysts is linked to a dynamic disparity between Fe-N and Fe-O bonds, causing Fe demetallization.
- The synthesized dual-Fe-atom catalyst exhibits a unique N3-Fe-Cl-Fe-N3 structure.
- The bridging Cl atom regulates electronic structure, enhancing Fe-N and Fe-Cl bond stability and attenuating Fe-O interactions during ORR.
- The catalyst demonstrated exceptional ORR stability, minimal Fe leaching (16.4 μg L-1 after 20000 cycles), retained 88% current over 160 h, and provided over 1000 h of stable performance in a zinc-air battery.
Conclusions:
- The study reveals the mechanism of Fe demetallization in Fe-N-C catalysts under ORR conditions.
- A dual-Fe-atom catalyst with a reinforced structure offers superior electrochemical robustness and durability.
- This work provides insights for designing highly stable, noble-metal-free ORR electrocatalysts.
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