Engineering highly selective CO2 electroreduction in Cu-based perovskites through A-site cation manipulation.
Shuaibing Yang1,2, Xiao-Min Chen1,2, Tao Shao2
1College of Chemistry, Fuzhou University, Fuzhou, 350108, P. R. China.
Physical Chemistry Chemical Physics : PCCP
|June 14, 2024
Summary
Doping perovskite oxides with Ce or Sr enhances electrocatalytic carbon dioxide reduction. This strategy improves methane and carbon monoxide production efficiencies by promoting key reaction intermediates and increasing active surface area.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Perovskite oxides show promise as catalysts but their use in CO2 reduction needs optimization.
- Understanding how to tune perovskite properties for enhanced CO2RR is crucial for developing efficient catalysts.
Purpose of the Study:
- To enhance the electrocatalytic activity of perovskite oxides for CO2 reduction.
- To investigate the effects of A-site ion doping (Ce and Sr) on La2CuO4 for CO2RR.
- To elucidate the mechanisms behind the improved catalytic performance.
Main Methods:
- Synthesis of Ce-doped La2CuO4 (LCCO) and Sr-doped La2CuO4 (LSCO) perovskite oxides.
- Electrochemical characterization including Faraday efficiency measurements at -1.4 V vs. RHE.
- In situ ATR-FTIR spectroscopy to identify reaction intermediates.
- XPS, EPR, and Cdl measurements to analyze material properties and active surface area.
Main Results:
- LCCO showed improved CH4 Faraday efficiency from 38.9% to 59.4%.
- LSCO demonstrated enhanced CO Faraday efficiency from 68.8% to 85.4%.
- Doping promoted the formation of *CHO and *HCOO intermediates and increased oxygen vacancies and electrochemical active surface area.
Conclusions:
- A-site ion doping is an effective strategy to enhance the CO2RR performance of perovskite oxides.
- The improved performance is attributed to the formation of key intermediates, increased oxygen vacancies, and higher electrochemical active surface area.
- This study provides insights into tuning perovskite catalysts for efficient CO2 conversion.
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