Self-supported NbSe2 nanosheet arrays for highly efficient ammonia electrosynthesis under ambient conditions

• Published in: Journal of catalysis Vol. 381; pp. 78 - 83
• Main Authors: Wang, Yong, Chen, Anran, Lai, Shuhua, Peng, Xianyun, Zhao, Shunzheng, Hu, Guangzhi, Qiu, Yuan, Ren, Junqiang, Liu, Xijun, Luo, Jun
• Format: Journal Article
• Language: English
• Published: Elsevier Inc 01.01.2020
• Subjects: 3D nanoarchitecture; N2 electroreduction; NbSe2 nanosheets; NH3 electrosynthesis; Self-supported; 3D nanoarchitecture; Self-supported; N2 electroreduction; NH3 electrosynthesis; NbSe2 nanosheets
• ISSN: 0021-9517; 1090-2694
• DOI: 10.1016/j.jcat.2019.10.029

[Display omitted] •NbSe2 NSA is firstly reported as an electrocatalyst for ambient NRR.•3D nanostructures of NbSe2 facilitate mass transport and exposure of active sites.•NbSe2 NSA can effectively actiate N2 molecules. As a promising alternative to the Haber–Bosch process for producing NH3, the electrocatalytic nitrogen reduction reaction (NRR) in the aqueous electrolyte has attracted much attention. However, the presence of sluggish reaction kinetics and competitive hydrogen evolution could result in poor activity and unsatisfactory selectivity. Herein, self-supported NbSe2 nanosheet arrays have been prepared and tested as electrocatalysts for NH3 electrosynthesis with a Faradaic efficiency of 13.9 ± 1.0% at −0.4 V versus the reversible hydrogen electrode (vs RHE) and a yield rate of 89.5 ± 6.0 μg h−1 mgcat.−1 at −0.45 V vs RHE in 0.1 M Na2SO4 under ambient conditions. Moreover, this electrocatalyst showed excellent durability during the 60-h electrolysis (no stable decay of Faradaic efficiencies and NH3 yield rates). Furthermore, density functional theory calculations disclosed that NbSe2 can effectively catalyze the dissociation of the adsorbed N2 molecule and thus promote the NRR process.