Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation. (18th January 2019)

• Record Type: Journal Article
• Authors: Han, Lili; Liu, Xijun; Chen, Jinping; Lin, Ruoqian; Liu, Haoxuan; Lü, Fang; Bak, Seongmin; Liang, Zhixiu; Zhao, Shunzheng; Stavitski, Eli; Luo, Jun; Adzic, Radoslav R.; Xin, Huolin L.
• Is Part Of: Angewandte Chemie. Volume 131:Number 8(2019)
• Page Start: 2343
• Page End: 2347
• Publication Date: 2019-01-18
• Subjects: Einzelatomkatalyse -- Elektrokatalyse -- Molybdän -- N2-Reduktion -- Umgebungsbedingungen; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.201811728
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: NH3 synthesis by the electrocatalytic N2 reduction reaction (NRR) under ambient conditions is an appealing alternative to the currently employed industrial method—the Haber–Bosch process—that requires high temperature and pressure. We report single Mo atoms anchored to nitrogen‐doped porous carbon as a cost‐effective catalyst for the NRR. Benefiting from the optimally high density of active sites and hierarchically porous carbon frameworks, this catalyst achieves a high NH3 yield rate (34.0±3.6 μg NH 3 h −1 mgcat. −1 ) and a high Faradaic efficiency (14.6±1.6 %) in 0.1 m KOH at room temperature. These values are considerably higher compared to previously reported non‐precious‐metal electrocatalysts. Moreover, this catalyst displays no obvious current drop during a 50 000 s NRR, and high activity and durability are achieved in 0.1 m HCl. The findings provide a promising lead for the design of efficient and robust single‐atom non‐precious‐metal catalysts for the electrocatalytic NRR. Abstract : Zusammen allein : Einzelne Molybdänatome, die auf N‐dotiertem, porösem Kohlenstoff verankert sind, wurden für die elektrokatalytische Reduktion von N2 zu NH3 entwickelt. Der Katalysator zeigt eine hohe elektrokatalytische Aktivität und Stabilität als Folge seiner Struktur, einen leitfähigen Kohlenstoffträger, hohe Porosität sowie gut dispergierte, einzelne Molybdänatome.