Details

Autor(en) / Beteiligte

• Meng, Zhe
• Yao, Jia‐Xin
• Sun, Chang‐Ning
• Kang, Xia
• Gao, Rui
• Li, Hong‐Rui
• Bi, Bo
• Zhu, Yong‐Fu
• Yan, Jun‐Min
• Jiang, Qing

Titel

Efficient Ammonia Production Beginning from Enhanced Air Activation

Ist Teil von

• Advanced energy materials, 2022-10, Vol.12 (38), p.n/a

Ort / Verlag

Weinheim: Wiley Subscription Services, Inc

Erscheinungsjahr

2022

Quelle

Wiley Online Library E-Journals

Beschreibungen/Notizen

• Ammonia is considered to be a next‐generation clean energy carrier, and thus the green synthesis of NH3 is of great importance. In this work, non‐thermal plasma oxidation is combined with electroreduction to achieve an efficient two‐step NH3 synthesis. A Ti bubbler is introduced in the first step of plasma activation of air to effectively produce nitrate/nitrite (NOx−) in an absorption solution, and the production rate achieves the highest value of 55.29 mmol h−1; the obtained NOx− aqueous solution is directly employed as catholyte for the second step of electroreduction with oxygen vacancy‐rich Co3O4 nanoparticles as the catalyst. Density functional theory calculations reveal that the introduction of oxygen vacancies endows their adjacent Co atoms with improved activity, which promotes adsorption and hydrogenation of NOx−, meanwhile suppressing the hydrogen evolution reaction. Thus the oxygen vacancy‐rich Co3O4 NPs present a significant NH3 production rate of 39.60 mg h−1 cm−2, high Faradaic efficiency of 96.08% and a large current density (376.48 mA cm−2), outperforming the previously reported ones including N2 or NOx− electroreduction. Efficient N2 reduction to NH3 is achieved by plasma‐assisted electroreduction. The NOx− production rate reaches 55.29 mmol h−1 under the synergistic effect of plasma and a bubbler. Subsequently, the Co3O4 NPs show excellent NOx− electroreduction performance with a high NH3 yield rate (39.60 mg h−1 cm−2) and Faradaic efficiency (96.08%) in a plasma‐generated NOx− (0.11 m) solution.