Recent advances in electrocatalytic NO<sub><i>x</i></sub> reduction into ammonia

Inta, Harish Reddy; Dhanabal, Dinesh; Markandaraj, Sridhar Sethuram; Shanmugam, Sangaraju

doi:10.1039/d3ey00090g

Cited by 4 publications

(2 citation statements)

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“…First, the N 2 evolution reaction was investigated via the mechanism outlined below (* denotes a surface site), which involves the adsorption of NO on the electrode surface, two sequential PCETs at the O atom, and the N–N coupling followed by N 2 desorption (eqs –). , 2 false( NO + * false) → 2 * NO 2 false( N * normalO + H + + e ‐ false) → 2 N * normalO normalH 2 false( N * normalO normalH + H + + e ‐ false) → 2 * normalN + 2 H 2 normalO 2 * normalN → N 2 + 2 * …”

Section: Results and Discussionmentioning

confidence: 99%

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Sustainable Electrosynthesis of Cyclohexanone Oxime through Nitrate Reduction on a Zn–Cu Alloy Catalyst

Sharp,

Ciotti,

Andrews

et al. 2024

ACS Catal.

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Cyclohexanone oxime is an important precursor for Nylon-6 and is typically synthesized via the nucleophilic addition−elimination of hydroxylamine with cyclohexanone. Current technologies for hydroxylamine production are, however, not environment-friendly due to the requirement of harsh reaction conditions. Here, we report an electrochemical method for the one-pot synthesis of cyclohexanone oxime under ambient conditions with aqueous nitrate as the nitrogen source. A series of Zn−Cu alloy catalysts are developed to drive the electrochemical reduction of nitrate, where the hydroxylamine intermediate formed in the electroreduction process can undergo a chemical reaction with the cyclohexanone present in the electrolyte to produce the corresponding oxime. The best performance is achieved on a Zn 93 Cu 7 electrocatalyst with a 97% yield and a 27% Faradaic efficiency for cyclohexanone oxime at 100 mA/cm 2 . By analyzing the catalytic activities/selectivities of the different Zn−Cu alloys and conducting in-depth mechanistic studies via in situ Raman spectroscopy and theoretical calculations, we demonstrate that the adsorption of nitrogen species plays a central role in catalytic performance. Overall, this work provides an attractive strategy to build the C−N bond in oxime and drive organic synthesis through electrochemical nitrate reduction, while highlighting the importance of controlling surface adsorption for product selectivity in electrosynthesis.

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Section: Results and Discussionmentioning

confidence: 99%

Section: Results and Discussionmentioning

confidence: 99%

Sustainable Electrosynthesis of Cyclohexanone Oxime through Nitrate Reduction on a Zn–Cu Alloy Catalyst

Sharp,

Ciotti,

Andrews

et al. 2024

ACS Catal.

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Construction of frustrated lewis pairs in ZnO surface for boosting electrocatalytic NO reduction to NH3: Theoretical prediction and experimental validation

Su,

Zhang,

Zhao

et al. 2024

Applied Catalysis B: Environment and Energy

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Tuning the electrocatalytic nitric oxide reduction activity of copper through alloying with nickel for NH₃ production at low overpotentials

Inta,

Dhanabal,

Song

et al. 2024

J. Mater. Chem. A

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Recent advances in electrocatalytic NO_x reduction into ammonia

Abstract: Ammonia (NH3) is an essential ingredient for the production of numerous chemicals which have a wider usage as fertilizers, explosives, and plastics. Currently, NH3 is mainly produced from the conventional...

Cited by 4 publications

References 116 publications

Sustainable Electrosynthesis of Cyclohexanone Oxime through Nitrate Reduction on a Zn–Cu Alloy Catalyst

Sustainable Electrosynthesis of Cyclohexanone Oxime through Nitrate Reduction on a Zn–Cu Alloy Catalyst

Construction of frustrated lewis pairs in ZnO surface for boosting electrocatalytic NO reduction to NH3: Theoretical prediction and experimental validation

Tuning the electrocatalytic nitric oxide reduction activity of copper through alloying with nickel for NH₃ production at low overpotentials

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Recent advances in electrocatalytic NOx reduction into ammonia

Abstract: Ammonia (NH3) is an essential ingredient for the production of numerous chemicals which have a wider usage as fertilizers, explosives, and plastics. Currently, NH3 is mainly produced from the conventional...

Cited by 4 publications

References 116 publications

Sustainable Electrosynthesis of Cyclohexanone Oxime through Nitrate Reduction on a Zn–Cu Alloy Catalyst

Sustainable Electrosynthesis of Cyclohexanone Oxime through Nitrate Reduction on a Zn–Cu Alloy Catalyst

Construction of frustrated lewis pairs in ZnO surface for boosting electrocatalytic NO reduction to NH3: Theoretical prediction and experimental validation

Tuning the electrocatalytic nitric oxide reduction activity of copper through alloying with nickel for NH3 production at low overpotentials

Contact Info

Product

Resources

About

Recent advances in electrocatalytic NO_x reduction into ammonia

Tuning the electrocatalytic nitric oxide reduction activity of copper through alloying with nickel for NH₃ production at low overpotentials