Ambient Electrochemical Nitrogen Fixation over a Bifunctional Mo–(O–C2)4 Site Catalyst
File version
Author(s)
Shi, T
Li, K
Sun, Q
Lin, Y
Zheng, LR
Wang, G
Zhang, Y
Yin, H
Zhang, H
Griffith University Author(s)
Primary Supervisor
Other Supervisors
Editor(s)
Date
Size
File type(s)
Location
License
Abstract
The electrochemical synthesis of NH3 and NO3- by the N2 reduction reaction (NRR) and the N2 oxidation reaction (NOR) under ambient conditions utilizing H2O as the hydrogen and oxygen source has aroused great attention. Here, we report the fabrication of oxygen-coordinated molybdenum (Mo) single atoms anchored on carbon (Mo-O-C) using bacterial cellulose (BC) as the impregnation regulator and carbon source. As a result, the as-synthesized Mo-O-C as an electrocatalyst exhibits superior bifunctional NRR and NOR activities with high stability. A superb NH3 yield rate of 248.6 ± 12.9 μg h-1 mgcat.-1 and a faradaic efficiency (FE) of 43.8 ± 2.3% can be obtained at -0.20 V (vs RHE) by the Mo-O-C-catalyzed NRR, and Mo-O-C can also afford a NO3- yield rate of 217.1 ± 13.5 μg h-1 mgcat.-1 with a FE of 7.8 ± 0.5% at 2.35 V (vs RHE) for the NOR. The synchrotron-based X-ray absorption spectra and theoretical calculation results unveil that the O-coordinated molybdenum configuration of Mo-(O-C2)4 anchored on carbon is the most stable single-atom structure as the catalytic active sites for N2 adsorption, activation, and bifunctional hydrogenation/oxidation reactions.
Journal Title
Journal of Physical Chemistry C
Conference Title
Book Title
Edition
Volume
126
Issue
2
Thesis Type
Degree Program
School
Publisher link
Patent number
Funder(s)
Grant identifier(s)
Rights Statement
Rights Statement
Item Access Status
Note
Access the data
Related item(s)
Subject
Catalysis and mechanisms of reactions
Physical chemistry
Persistent link to this record
Citation
Zhang, S; Shi, T; Li, K; Sun, Q; Lin, Y; Zheng, LR; Wang, G; Zhang, Y; Yin, H; Zhang, H, Ambient Electrochemical Nitrogen Fixation over a Bifunctional Mo–(O–C2)4 Site Catalyst, Journal of Physical Chemistry C, 2021, 126 (2), pp. 965-973