Spontaneous Atomic Ruthenium Doping in Mo2CTX MXene Defects Enhances Electrocatalytic Activity for the Nitrogen Reduction Reaction

The electrochemical nitrogen reduction reaction (NRR) process usually suffers extremely low Faradaic efficiency and ammonia yields due to sluggish NN dissociation. Herein, single‐atomic ruthenium modified Mo2CTX MXene nanosheets as an efficient electrocatalyst for nitrogen fixation at ambient condi...

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Bibliographic Details
Published in:Advanced energy materials 2020-07, Vol.10 (25), p.n/a
Main Authors: Peng, Wei, Luo, Min, Xu, Xiandong, Jiang, Kang, Peng, Ming, Chen, Dechao, Chan, Ting‐Shan, Tan, Yongwen
Format: Article
Language:English
Subjects:
Ammonia
Catalysts
Chemical reduction
Density functional theory
doping
Electrocatalysts
electrocatalytic nitrogen reduction
Hydrogen storage
MXene
MXenes
Nanostructure
Nitrogen
Nitrogenation
Potassium sulfate
Ruthenium
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Summary:The electrochemical nitrogen reduction reaction (NRR) process usually suffers extremely low Faradaic efficiency and ammonia yields due to sluggish NN dissociation. Herein, single‐atomic ruthenium modified Mo2CTX MXene nanosheets as an efficient electrocatalyst for nitrogen fixation at ambient conditions are reported. The catalyst achieves a Faradaic efficiency of 25.77% and ammonia yield rate of 40.57 µg h−1 mg−1 at ‐0.3 V versus the reversible hydrogen electrode in 0.5 m K2SO4 solution. Operando X‐ray absorption spectroscopy studies and density functional theory calculations reveal that single‐atomic Ru anchored on MXene nanosheets act as important electron back‐donation centers for N2 activation, which can not only promote nitrogen adsorption and activation behavior of the catalyst, but also lower the thermodynamic energy barrier of the first hydrogenation step. This work opens up a promising avenue to manipulate catalytic performance of electrocatalysts utilizing an atomic‐level engineering strategy. Single‐atomic ruthenium modified Mo2CTX MXene nanosheets are developed as an efficient electrocatalyst for nitrogen fixation under ambient conditions. The catalyst achieves a high Faradaic efficiency and a large ammonia yield rate in 0.5 m K2SO4 solution, outperforming many previous reported nitrogen reduction reaction electrocatalysts. The high activity and durability enable the single‐atomic Ru‐Mo2CTX to be a promising electrocatalyst for artificial nitrogen fixation.
ISSN:1614-6832
1614-6840
DOI:10.1002/aenm.202001364