Modulating the Nitrate Reduction Pathway on Unconventional Phase Ultrathin Nanoalloys for Selective Ammonia
Jingwen Zhou1,2, Fu Liu1, Zhihang Xu3
1Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong SAR 999077, China.
Journal of the American Chemical Society
|June 20, 2025
Summary
This study introduces a novel 2H-RhCu catalyst for efficient ammonia (NH3) electrosynthesis from nitrate wastewater. The engineered catalyst demonstrates superior selectivity and yield, offering a promising solution for green chemistry and sewage treatment.
Area of Science:
- Electrochemistry
- Materials Science
- Environmental Engineering
Background:
- Ammonia (NH3) electrosynthesis from nitrate wastewater is crucial for sustainable chemical production and wastewater treatment.
- Key challenges include achieving high selectivity, low overpotential, and rapid nitrate reduction reaction (NO3RR) rates.
Purpose of the Study:
- To enhance neutral NO3RR performance using a dual engineering strategy involving catalyst crystal phase and electrode/electrolyte interface.
- To investigate the effectiveness of ultrathin alloy nanostructures, specifically the unconventional 2H-RhCu phase.
Main Methods:
- Fabrication of ultrathin alloy nanostructures with engineered crystal phases (2H-RhCu).
- Electrocatalytic testing in various electrolytes (K+, Li+, Na+) to evaluate NH3 selectivity and efficiency.
- In situ studies and theoretical calculations to elucidate reaction mechanisms and interfacial effects.
Main Results:
- The 2H-RhCu catalyst exhibited higher intrinsic NH3 selectivity compared to traditional phases.
- Superior Faradaic efficiency and yield rate for NH3 production were observed in a K+-based electrolyte.
- Identified enhanced kinetics, reduced N-N recombination, and unique *NObri adsorption as key factors for improved performance.
Conclusions:
- The dual engineering strategy effectively enhances neutral NO3RR performance.
- 2H-RhCu presents a promising catalyst for efficient and selective ammonia electrosynthesis.
- Demonstrated potential applications in rechargeable Zn-nitrate/methanol flow batteries.
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