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Ammonia Synthesis at Low Pressure
Published on: August 23, 2017
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Ammonia Electrosynthesis from Nitrate Using a Ruthenium-Copper Cocatalyst System: A Full Concentration Range Study.
Qikun Hu1, Ke Yang2, Ouwen Peng1
1Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Singapore.
Journal of the American Chemical Society
|December 28, 2023
Summary
Electrochemical ammonia synthesis from concentrated nitrate waste is now possible using a Ru/Cu2O catalyst. This breakthrough addresses poor hydrogen transfer kinetics, enabling efficient ammonia production in flow electrolyzers.
Area of Science:
- Electrochemistry
- Catalysis
- Materials Science
Background:
- Electrochemical synthesis of ammonia (electrochemical ammonia synthesis) via the nitrate reduction reaction (NO3RR) is a promising alternative to the Haber-Bosch process.
- Research has primarily focused on low nitrate concentrations, neglecting high-concentration waste streams from nuclear and fertilizer industries.
- High electrolyte concentrations (≥1 M) required for efficient production are limited by slow hydrogen transfer kinetics.
Purpose of the Study:
- To develop a cocatalytic system for efficient electrochemical ammonia synthesis from concentrated nitrate solutions.
- To investigate the mechanism of hydrogen transfer and identify key intermediates in the NO3RR process.
- To overcome the kinetic bottleneck in electrosynthesis for high-rate ammonia production.
Main Methods:
- Utilized a cocatalytic system of Ruthenium (Ru) and Copper(I) oxide (Cu2O) catalyst.
- Conducted experiments in a 16 cm2 flow electrolyzer with a 1 M nitrate electrolyte.
- Employed deuterium labeling and operando Fourier transform infrared (FTIR) spectroscopy for mechanistic studies.
- Performed ab initio molecular dynamics (AIMD) simulations to understand hydrogen transfer mechanisms.
Main Results:
- Achieved NO3RR at 10.0 A with 100% faradaic efficiency toward ammonia production.
- Identified that adsorbed hydroxide on Ru nanoparticles enhances the hydrogen-bonded water network near the Cu2O surface.
- Demonstrated a promoted hydrogen transfer rate due to synergistic interactions between Ru and Cu2O.
Conclusions:
- The Ru/Cu2O cocatalyst system effectively enables high-rate electrochemical ammonia synthesis from concentrated nitrate electrolytes.
- Synergistic interactions between catalyst components are crucial for overcoming kinetic limitations in electrosynthesis.
- This work provides a pathway for valorizing concentrated nitrate waste streams through efficient ammonia production.
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