Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 57, Issue 39, Pages 14558-14568Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.3c05443
Keywords
DBD plasma; electrocatalytic reduction; synthesisof ammonia; sustainable ammonia production
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This paper proposes a cascade N-2 reduction process for ammonia synthesis using dielectric barrier discharge (DBD) plasma oxidation and electrocatalytic reduction. N-2 is oxidized to reactive nitrogen species (RNS) by nonthermal plasma and then electroreduced to NH4+. The study demonstrates high selectivity and yield of ammonia using a cobalt catalyst in the electrocatalytic reduction process.
Due to the extremely high bond energy of N equivalent to N (similar to 941 kJ/mol), the traditional Haber-Bosch process of ammonia synthesis is known as an energy-intensive and high CO2-emission industry. In this paper, a cascade N-2 reduction process with dielectric barrier discharge (DBD) plasma oxidation and electrocatalytic reduction as an alternative route is first proposed. N-2 is oxidized to be reactive nitrogen species (RNS) by nonthermal plasma, which would then be absorbed by KOH solution and electroreduced to NH4+. It is found that the production of NOx is a function of discharge length, discharge power, and gas flow rate. Afterward, the cobalt catalyst is used in the process of electrocatalytic reduction of ammonia, which shows high selectivity (Faradic efficiency (FE) above 90%) and high yield of ammonia (45.45 mg/h). Finally, the cascade plasma oxidation and electrocatalytic reduction for ammonia synthesis is performed. Also, the performance of the reaction system is evaluated. It is worth mentioning that a stable and sustainable ammonia production efficiency of 16.21 mg/h is achieved, and 22.16% of NOx obtained by air activation is converted into NH4+. This work provides a demonstration for further industrial application of ammonia production with DBD plasma oxidation and electrocatalytic reduction techniques.
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