Details

Autor(en) / Beteiligte

• Wan, Yuying
• Zhang, Ying
• Zhang, Nana
• Zhang, Zhuoyan
• Chu, Ke

Titel

Single-atom Zn on MnO2 for selective nitrite electrolysis to ammonia

Ist Teil von

• Chemical engineering journal (Lausanne, Switzerland : 1996), 2024-02, Vol.481, p.148734, Article 148734

Ort / Verlag

Elsevier B.V

Erscheinungsjahr

2024

Quelle

Access via ScienceDirect (Elsevier)

Beschreibungen/Notizen

• [Display omitted] •Single-atom Zn on MnO2 (Zn1/MnO2) is explored as an efficient NO2RR catalyst.•Zn1/MnO2-flow cell shows an FENH3 of 95.3 % and NH3 yield of 1559.1 μmol h−1cm−2.•Zn1-O3 units on Zn1/MnO2 can activate NO2− and accelerate the NO2RR energetics. Electrochemical nitrite-to-ammonia reduction (NO2RR) represents an attractive method to simultaneously attain hazardous NO2− removal and renewable NH3 synthesis. In this study, we first design single-atom Zn anchored on MnO2 nanowires (Zn1/MnO2) as a highly active and durable NO2RR catalyst. Atomic-scale characterizations reveal that Zn single atoms are coordinated with three surface-O atoms of MnO2 to form Zn1-O3 units. A combination of in situ electrochemical measurements and theoretical computations unravel that Zn1-O3 units enhance the NO2− activation, stabilize the key intermediate of *NHO and lower the energy barrier of NO2−-to-NH3 hydrogenation process. Consequently, Zn1/MnO2 assembled in a special flow cell reactor achieves the highest NH3 yield rate of 1559.1 μmol h−1cm−2 and NH3-Faradaic efficiency of 95.3 % at −288.5 mA cm−2, superior to nearly all previously reported NO2RR electrocatalysts.