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Metal-organic framework derived single-atom catalysts for electrochemical CO2 reduction
Mengna Xie1,2, Jiawei Wang1,2, Xian-Long Du1,3,4
1Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences Shanghai 201800 China duxianlong@sinap.ac.cn.
Transition metal single atom catalysts (SACs) effectively convert CO2 to CO. Fe-N-C catalysts, synthesized via ZIF pyrolysis, show superior performance in electrochemical CO2 reduction, achieving high CO selectivity.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Electrochemical reduction of carbon dioxide (CO2) to carbon monoxide (CO) is a key process for sustainable energy.
- Transition metal single atom catalysts (SACs) offer high atomic utilization and catalytic efficiency.
- Metal-nitrogen-carbon (M-N-C) materials are promising supports for SACs in CO2 reduction reactions (CO2RR).
Purpose of the Study:
- To construct and investigate a series of M-N-C based SACs for CO2RR.
- To evaluate the catalytic performance of different transition metals (Fe, Ni, Mn, Co, Cu) within the M-N-C framework.
- To optimize the synthesis of Fe-N-C catalysts by studying the effect of pyrolysis temperature on CO2RR activity and selectivity.
Main Methods:
- Facile pyrolysis of zeolitic imidazolate frameworks (ZIFs) to create M-N-C SACs.
- X-ray photoelectron spectroscopy (XPS) for chemical state and M-N bonding analysis.
- High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) for morphological and distribution analysis.
- Electrochemical CO2 reduction reaction (CO2RR) testing to assess catalytic performance.
Main Results:
- Successfully synthesized M-N-C based SACs with metal single atoms on nitrogen-doped carbon supports.
- XPS confirmed the presence of M-N coordination bonds, crucial for catalytic activity.
- HAADF-STEM demonstrated homogeneous distribution of metal single atoms.
- Fe-N-C catalyst exhibited the highest activity and nearly 100% faradaic efficiency for CO (FE_CO) at -0.9 V vs. RHE.
- Fe-N-C catalyst pyrolyzed at 1000 °C showed optimal CO2RR performance and selectivity.
Conclusions:
- M-N-C based SACs, particularly Fe-N-C, are highly effective for electrochemical CO2RR.
- The M-N coordination and nitrogen-doped carbon support play critical roles in catalytic performance.
- Optimized pyrolysis temperature is essential for maximizing the activity and selectivity of Fe-N-C catalysts for CO production.
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