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Engineering Atomic Single Metal-FeN4Cl Sites with Enhanced Oxygen-Reduction Activity for High-Performance Proton
Shichao Ding1, Jordan Alysia Barr1, Qiurong Shi2
1School of Mechanical and Materials Engineering, Washington State University, Pullman, Washington 99164, United States.
ACS Nano
|September 12, 2022
Summary
Chlorine doping enhances iron-nitrogen-carbon single-atomic site catalysts (Fe-N-C SACs) for the oxygen reduction reaction (ORR). This novel approach improves catalytic activity in fuel cells compared to traditional Fe-N-C SACs.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Iron-nitrogen-carbon single-atomic site catalysts (Fe-N-C SACs) are promising alternatives to platinum for oxygen reduction reaction (ORR) in proton exchange membrane fuel cells.
- Current strategies to enhance Fe-N-C SACs often involve heteroatom doping, but typically result in uncontrolled long-range interactions, limiting precise modulation of the active sites.
- Developing methods for controlled near-range interactions is crucial for optimizing the electronic structure and catalytic performance of Fe-N-C SACs.
Purpose of the Study:
- To investigate the effect of chlorine (Cl) doping on the Fe-N-C active center for enhanced ORR activity.
- To explore the use of near-range coordinated interactions for precise electronic structure modulation in SACs.
- To evaluate the performance of Cl-doped Fe-N-C SACs in proton exchange membrane fuel cells.
Main Methods:
- Synthesis of a novel FeN4Cl single-atomic site catalyst.
- Characterization of the catalyst structure and active sites.
- Density functional theory (DFT) calculations to understand electronic structure modifications.
- Electrochemical evaluation of ORR activity using half-wave potential (E1/2) measurements.
- Testing catalyst performance in membrane electrode assemblies (MEAs).
Main Results:
- Successful synthesis of FeN4Cl SACs with likely FeN4Cl active sites within a carbon matrix.
- DFT calculations confirmed improved intrinsic ORR activity due to Fe-Cl coordination.
- Experimental results showed a significantly enhanced ORR half-wave potential of 0.818 V.
- The FeN4Cl SAC demonstrated excellent performance in membrane electrode assembly tests.
Conclusions:
- Near-range coordinated interaction using chlorine doping effectively modulates the Fe-N active center in Fe-N-C SACs.
- The Fe-Cl coordination enhances the intrinsic ORR activity compared to undoped Fe-N SACs.
- The developed FeN4Cl SAC shows great potential for efficient and durable oxygen reduction reaction catalysis in fuel cells.
