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Sulfate-Enabled Nitrate Synthesis from Nitrogen Electrooxidation on a Rhodium Electrocatalyst
Tieliang Li1, Shuhe Han1, Chuanqi Cheng2
1Institute of Molecular Plus, Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.
Angewandte Chemie (International Ed. in English)
|April 20, 2022
Summary
Sulfate enhances the electrocatalytic nitrogen oxidation reaction (NOR) over Rh catalysts. This method efficiently converts nitrogen to nitrate, overcoming challenges associated with the strong nitrogen-nitrogen triple bond.
Area of Science:
- Electrochemistry
- Catalysis
- Green Chemistry
Background:
- Electrocatalytic nitrogen oxidation reaction (NOR) offers a sustainable alternative to industrial nitrate production.
- The strong nitrogen-nitrogen triple bond (941 kJ mol⁻¹) presents a significant challenge for NOR.
- Current electrocatalysts struggle with efficient nitrogen activation and conversion.
Purpose of the Study:
- To investigate the use of sulfate as a promoter for enhancing NOR performance.
- To improve the efficiency of nitrate generation via electrocatalytic nitrogen oxidation.
- To understand the mechanism by which sulfate enhances the reaction over Rh catalysts.
Main Methods:
- Electrochemical synthesis of nitrate from nitrogen using an Rh electrocatalyst.
- Addition of sulfate to the electrolyte to study its effect on NOR.
- In situ electrochemical characterizations and theoretical calculations.
- 15N isotope-labeling experiments to confirm nitrate origin.
Main Results:
- Sulfate addition significantly enhanced NOR performance over Rh nanoparticles.
- Achieved a high nitrate yield of 168.0 μmol g_cat⁻¹ h⁻¹.
- Confirmed nitrate production from nitrogen electrooxidation using 15N labeling.
- Sulfate promotes nitrogen adsorption and lowers the reaction energy barrier.
Conclusions:
- Sulfate acts as an effective promoter for electrocatalytic nitrogen oxidation.
- In situ generated sulfate radicals reduce the activation energy of the rate-determining step.
- This study presents a promising strategy for efficient and sustainable nitrate synthesis.
Keywords:
15N Isotope LabelingArtificial Nitrogen FixationIn Situ Multiple CharacterizationsN2 ElectrooxidationSulfateMore Related Videos
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