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A Copper-Zinc Cyanamide Solid-Solution Catalyst with Tailored Surface Electrostatic Potentials Promotes Asymmetric
Jiacheng Jayden Wang1,2, Huong T D Bui3, Xunlu Wang4
1The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China.
Journal of the American Chemical Society
|February 18, 2025
Summary
This study introduces a novel copper-zinc cyanamide catalyst for efficient electrocatalytic nitrite reduction, converting pollutants into valuable ammonia with high selectivity and activity under ambient conditions.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Electrocatalytic nitrite reduction (NO2RR) offers a sustainable route to ammonia (NH3) production from nitrogenous pollutants.
- Current NO2RR electrocatalysts suffer from low activity and NH3 selectivity due to complex reaction intermediates and proton transfer processes.
Purpose of the Study:
- To develop a novel solid-solution copper-zinc cyanamide (Cu0.8Zn0.2NCN) catalyst for enhanced NO2RR.
- To investigate the mechanism of improved NO2RR performance through tailored surface electrostatic potential and asymmetric NO2- binding.
Main Methods:
- Synthesis of solid-solution Cu0.8Zn0.2NCN.
- Electrocatalytic performance evaluation for NO2RR.
- In situ spectroscopic measurements and theoretical calculations to elucidate the reaction mechanism.
Main Results:
- Cu0.8Zn0.2NCN exhibited outstanding NO2RR performance with ~100% Faradaic efficiency and 22 mg h-1 cm-2 NH3 yield.
- Theoretical and experimental data revealed that Cu-Zn sites with linear polarized [NCN]2- promote asymmetric NO2- binding and enhance adsorption/bond cleavage.
- A paired electro-refinery demonstrated stable operation at industrial-level current densities (>400 mA cm-2) for over 140 hours.
Conclusions:
- Solid-solution strategy effectively tailors surface electrostatic potential for advanced electrocatalysis.
- Cu0.8Zn0.2NCN presents a promising material for efficient and selective electrocatalytic ammonia synthesis from nitrite.
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