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Updated: May 28, 2025
Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
Planar chlorination engineering induced symmetry-broken single-atom site catalyst for enhanced CO2 electroreduction
Shengjie Wei1,2, Jiexin Zhu3,4, Xingbao Chen5
1Center Excellence for Environmental Safety and Biological Effects, Beijing Key Laboratory for Green Catalysis and Separation, Department of Chemistry, College of Chemistry and Life Science, Beijing University of Technology, Beijing, 100124, China.
Planar chlorination engineering transforms low-activity Zn-N4 sites into highly active Zn-N3 sites for efficient carbon dioxide reduction (CO2RR). This breakthrough enhances catalytic performance and stability for industrial applications.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Traditional metal-N4 sites often exhibit limited activity and selectivity in CO2RR.
- Breaking geometric symmetry is crucial for enhancing catalytic performance.
- Developing efficient catalysts for CO2 reduction is vital for sustainable chemistry.
Purpose of the Study:
- To engineer Zn-N4 sites into a lower-coordination Zn-N3 structure.
- To investigate the effect of planar chlorination on CO2RR activity.
- To develop a highly active and stable catalyst for CO2 reduction.
Main Methods:
- Planar chlorination engineering of Zn-N4 sites.
- Electrochemical characterization including CO2 reduction reaction (CO2RR) tests.
- In-situ extended X-ray absorption fine structure (EXAFS) and density functional theory (DFT) calculations.
Main Results:
- The optimized catalyst (Zn-SA/CNCl-1000) achieved a high FECO of 97% and stability over 50 hours at 200 mA/cm2.
- The Zn-N3 sites with broken symmetry significantly boosted CO partial current density (271.7 mA/cm2) and TOF (29325 h-1).
- C-Cl bond induced self-reconstruction of Zn-N4 to Zn-N3 sites, strengthening *COOH adsorption.
Conclusions:
- Planar chlorination is an effective strategy to break geometric symmetry and enhance catalytic activity.
- The novel Zn-N3 sites demonstrate superior performance in CO2RR compared to traditional Zn-N4 sites.
- This work offers a promising pathway for designing advanced catalysts for industrial CO2 utilization.
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