Electrocatalytic Nitrate and Nitrite Reduction toward Ammonia using Cu2O 
Nanocubes: Active Species and Reaction Mechanisms

Bai, Lichen; Franco, Federico; Timoshenko, Janis; Rettenmaier, Clara; Scholten, Fabian; Jeon, Hyosang; Yoon, Aram; Rüscher, Martina; Herzog, Antonia; Haase, Felix; Kühl, Stefanie; Chee, See Wee; Bergmann, Arno; Roldan Cuenya, Beatriz

doi:10.1021/jacs.3c13288

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Electrocatalytic Nitrate and Nitrite Reduction toward Ammonia using Cu₂O Nanocubes: Active Species and Reaction Mechanisms

MPG-Autoren

/persons/resource/persons271029

Bai, Lichen
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons232505

Franco, Federico
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227619

Timoshenko, Janis
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227610

Rettenmaier, Clara
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227612

Scholten, Fabian
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227603

Jeon, Hyosang
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons244720

Yoon, Aram
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons267176

Rüscher, Martina
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons232519

Herzog, Antonia
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227601

Haase, Felix
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21771

Kühl, Stefanie
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons244748

Chee, See Wee
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons214068

Bergmann, Arno
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22020

Roldan Cuenya, Beatriz
Interface Science, Fritz Haber Institute, Max Planck Society;

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Zitation

Bai, L., Franco, F., Timoshenko, J., Rettenmaier, C., Scholten, F., Jeon, H., et al. (2024). Electrocatalytic Nitrate and Nitrite Reduction toward Ammonia using Cu₂O Nanocubes: Active Species and Reaction Mechanisms. Journal of the American Chemical Society, 146(14), 9665-9678. doi:10.1021/jacs.3c13288.

Zitierlink: https://hdl.handle.net/21.11116/0000-000E-B34A-5

Zusammenfassung

The electrochemical reduction of nitrate (NO3–) and nitrite (NO2–) enables sustainable, carbon-neutral, and decentralized routes to produce ammonia (NH3). Copper-based materials are promising electrocatalysts for NOx– conversion to NH3. However, the underlying reaction mechanisms and the role of different Cu species during the catalytic process are still poorly understood. Herein, by combining quasi in situ X-ray photoelectron spectroscopy (XPS) and operando X-ray absorption spectroscopy (XAS), we unveiled that Cu is mostly in metallic form during the highly selective reduction of NO3–/NO2– to NH3. On the contrary, Cu(I) species are predominant in a potential region where the two-electron reduction of NO3– to NO2– is the major reaction. Electrokinetic analysis and in situ Raman spectroscopy was also used to propose possible steps and intermediates leading to NO2– and NH3, respectively. This work establishes a correlation between the catalytic performance and the dynamic changes of the chemical state of Cu, and provides crucial mechanistic insights into the pathways for NO3–/NO2– electrocatalytic reduction.