Electrocatalytic Hydrogenation of N2 to NH3 by MnO: Experimental and Theoretical Investigations. Issue 1 (9th November 2018)

• Record Type: Journal Article
• Authors: Wang, Zao; Gong, Feng; Zhang, Ling; Wang, Rui; Ji, Lei; Liu, Qian; Luo, Yonglan; Guo, Haoran; Li, Yuehui; Gao, Peng; Shi, Xifeng; Li, Baihai; Tang, Bo; Sun, Xuping
• Is Part Of: Advanced science. Volume 6:Issue 1(2019)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2018-11-09
• Subjects: ambient conditions -- artificial N2 fixation -- electrocatalysis -- MnO -- NH3; Science -- Periodicals; 505
• DOI: 10.1002/advs.201801182
• Languages: English
• ISSNs: 2198-3844

Abstract

Abstract: NH3 is a valuable chemical with a wide range of applications, but the conventional Haber–Bosch process for industrial‐scale NH3 production is highly energy‐intensive with serious greenhouse gas emission. Electrochemical reduction offers an environmentally benign and sustainable route to convert N2 to NH3 at ambient conditions, but its efficiency depends greatly on identifying earth‐abundant catalysts with high activity for the N2 reduction reaction. Here, it is reported that MnO particles act as a highly active catalyst for electrocatalytic hydrogenation of N2 to NH3 with excellent selectivity. In 0.1m Na2 SO4, this catalyst achieves a high Faradaic efficiency up to 8.02% and a NH3 yield of 1.11 × 10 −10 mol s −1 cm −2 at −0.39 V versus reversible hydrogen electrode, with great electrochemical and structural stability. On the basis of density functional theory calculations, MnO (200) surface has a smaller adsorption energy toward N than that of H with the *N2 → *N2 H transformation being the potential‐determining step in the nitrogen reduction reaction. Abstract : A manganese oxide particles film on Ti mesh (MnO/TM) acts as a robust non‐noble‐metal electrocatalyst for efficient N2 reduction electrocatalysis at ambient conditions. In 0.1m Na2 SO4, the MnO/TM attains a high Faradaic efficiency up to 8.02% and a NH3 yield of 1.11 × 10 −10 mol s −1 cm −2 at −0.39 V versus reversible hydrogen electrode, with high electrochemical stability.