Details

Autor(en) / Beteiligte

• Shen, Zhen
• Yu, Yingsong
• Zhao, Zhiwei
• Mushtaq, Muhammad Asim
• Ji, Qianqian
• Yasin, Ghulam
• Rehman, Lashari Najeeb Ur
• Liu, Xiaochun
• Cai, Xingke
• Tsiakaras, Panagiotis
• Zhao, Jie

Titel

N, O trans-coordinating silver single-atom catalyst for robust and efficient ammonia electrosynthesis from nitrate

Ist Teil von

• Applied catalysis. B, Environmental, 2023-08, Vol.331, p.122687, Article 122687

Ort / Verlag

Elsevier B.V

Erscheinungsjahr

2023

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Single-atom catalysts (SACs) containing noble metals have been largely explored for various catalytic reactions and demonstrated high activity and chemical stability but are rarely used for electrocatalytic nitrate reduction to ammonia (NO3−RA) because of their strong tendency towards hydrogen evolution reaction (HER). Herein, we developed the N, O trans-coordination strategy to inhibit the HER of carbon nanotube-based Ag SACs (Ag1/NOCNT) catalyst, thus improving the NH3 production. The Ag1/NOCNT exhibits a record-high ammonia yield rate (YRNH3) of 90 mol h−1 gAg−1, more than two folds of the best-reported SACs using carbon supports, as well as high Faradaic efficiency (FENH3) of 97.9% and optimal electrochemical stability. These excellent performances attribute to the novel trans AgN2O2 configuration, suppressing the HER, optimizing the adsorption of intermediates and facilitating the potential-determining step in NO3−RA. The corresponding plasma-driven nitrogen oxidation and NOx− reduction coupling system presented high YRNH3 of ∼1.3 mol h−1 g−1 (∼41.5 mol h−1 gAg−1) and FENH3 of 85.2%, demonstrating high feasibility for sustainable green NH3 synthesis over specially designed catalytic materials under ambient conditions. [Display omitted] •The Ag single-atom catalysts (SACs) with N, O trans coordination were reported.•The novel catalyst presented a record-high NH3 yield rate among carbon-based SACs.•The trans AgN2O2 configuration played a key role in improving NH3 production.•The practical-sustainable NH3 synthesis was demonstrated by a pNO–NOx−RA system.