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Plasma-assisted defect engineering of N-doped NiCo2O4 for efficient oxygen reduction
Jingxuan Zheng1, Xiangfeng Peng, Zhao Wang
1National Engineering Research Centre of Industry Crystallization Technology, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China. wangzhao@tju.edu.cn.
Physical Chemistry Chemical Physics : PCCP
|March 11, 2021
Summary
Cold plasma treatment enhances NiCo2O4 electrocatalysis for oxygen reduction reactions (ORR) by creating oxygen vacancies and doping nitrogen. This improves catalyst conductivity and stability, leading to superior ORR performance.
Area of Science:
- Materials Science
- Electrochemistry
- Surface Science
Background:
- Defect control in metal oxides is crucial for enhancing electrocatalysis.
- Oxygen vacancies and nitrogen doping are effective strategies to improve catalyst performance.
- Nickel cobaltate (NiCo2O4) is a promising electrocatalyst material.
Purpose of the Study:
- To prepare oxygen vacancy-enriched and nitrogen-doped NiCo2O4 using cold plasma.
- To investigate the effect of plasma treatment on the electrocatalytic performance for the oxygen reduction reaction (ORR).
- To elucidate the mechanism behind the enhanced ORR activity.
Main Methods:
- Synthesis of NiCo2O4 using cold plasma with oxygen as the plasma-forming gas.
- Controlled introduction of oxygen vacancies and nitrogen doping.
- Electrocatalytic performance evaluation for ORR.
- Density Functional Theory (DFT) calculations.
Main Results:
- Successfully prepared oxygen vacancy-enriched NiCo2O4 with controlled vacancy concentration.
- Achieved high nitrogen doping (up to 10.1%) on NiCo2O4.
- Plasma-treated NiCo2O4 exhibited enhanced ORR activity with a typical four-electron pathway.
- Achieved low HO2- byproduct formation (0.59%) and high current density (4.9 mA cm-2 at 0.2 V).
- DFT calculations revealed increased electron density, reduced work function, and shifted d-band center.
Conclusions:
- Cold plasma treatment is an effective method for creating oxygen vacancies and doping nitrogen into NiCo2O4.
- The resulting N-doped NiCo2O4 demonstrates significantly improved electrocatalytic performance for ORR.
- Plasma-induced modifications enhance charge transfer, conductivity, and catalytic activity, offering a promising route for advanced electrocatalyst design.
