Boosting Electrochemical Nitrogen Fixation via Regulating Surface Electronic Structure by CeO2 Hybridization
Bin Fang1, Xiao Wang1,2, Shuaishuai Zhang1
1State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China.
Small (Weinheim an Der Bergstrasse, Germany)
|January 9, 2024
Summary
This study introduces advanced electrocatalysts for sustainable ammonia production via nitrogen reduction reaction (NRR). The novel CeO2-MoN catalyst achieves high ammonia yield and selectivity, offering a promising route for green ammonia synthesis.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Electrocatalytic nitrogen reduction reaction (NRR) is a sustainable method for ammonia (NH3) production.
- Current NRR catalysts suffer from low NH3 yield and poor selectivity.
- Developing high-performance NRR catalysts and understanding structure-performance relationships are crucial.
Purpose of the Study:
- To develop advanced catalysts for efficient electrocatalytic nitrogen reduction reaction (NRR).
- To investigate the structure-performance relationship of novel catalysts for ammonia synthesis.
Main Methods:
- A molten-salt approach was used to synthesize cerium dioxide (CeO2) nanoparticles anchored by molybdenum nitride (MoN) nanosheets.
- Electrocatalytic performance was evaluated for ammonia production under ambient conditions.
- Experimental analysis and density functional theory (DFT) calculations were employed to understand the catalytic mechanism.
Main Results:
- The synthesized CeO2-MoN catalyst achieved a high NH3 yield rate of 27.5 µg h⁻¹ mg⁻¹ and a Faradaic efficiency of 17.2% at -0.3 V vs RHE.
- DFT calculations revealed that MoN incorporation in CeO2 enlarges the electron-deficient area of nitrogen vacancies.
- This enhancement facilitates N2 adsorption/activation and the generation of key intermediates, boosting NRR performance.
Conclusions:
- The CeO2-MoN nanocomposite demonstrates excellent performance as an electrocatalyst for NRR.
- The enlarged electron-deficient sites are key to improving N2 activation and ammonia synthesis.
- This work provides a promising strategy for designing efficient catalysts for green ammonia production.
