Enhanced NH3 Synthesis from Air in a Plasma Tandem- Electrocatalysis System Using Plasma-Engraved N-Doped Defective MoS2

Zheng, Jiageng, Zhang, Hao, Lv, Jiabao, Zhang, Meng, Wan, Jieying, Gerrits, Nick, Wu, Angjian, Lan, Bingru, Wang, Weitao, Wang, Shuangyin
et al (show 3 more authors) (2023) Enhanced NH3 Synthesis from Air in a Plasma Tandem- Electrocatalysis System Using Plasma-Engraved N-Doped Defective MoS2. JACS AU, 3 (5). pp. 1328-1336.

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We have developed a sustainable method to produce NH<sub>3</sub> directly from air using a plasma tandem-electrocatalysis system that operates via the N<sub>2</sub>-NO<sub><i>x</i></sub>-NH<sub>3</sub> pathway. To efficiently reduce NO<sub>2</sub><sup>-</sup> to NH<sub>3</sub>, we propose a novel electrocatalyst consisting of defective N-doped molybdenum sulfide nanosheets on vertical graphene arrays (N-MoS<sub>2</sub>/VGs). We used a plasma engraving process to form the metallic 1T phase, N doping, and S vacancies in the electrocatalyst simultaneously. Our system exhibited a remarkable NH<sub>3</sub> production rate of 7.3 mg h<sup>-1</sup> cm<sup>-2</sup> at -0.53 V vs RHE, which is almost 100 times higher than the state-of-the-art electrochemical nitrogen reduction reaction and more than double that of other hybrid systems. Moreover, a low energy consumption of only 2.4 MJ mol<sub>NH<sub>3</sub></sub><sup>-1</sup> was achieved in this study. Density functional theory calculations revealed that S vacancies and doped N atoms play a dominant role in the selective reduction of NO<sub>2</sub><sup>-</sup> to NH<sub>3</sub>. This study opens up new avenues for efficient NH<sub>3</sub> production using cascade systems.

Item Type: Article
Uncontrolled Keywords: sustainable NH3 production, plasma electrocatalysis, defective N-MoS2, plasma engraving, density functional theory
Divisions: Faculty of Science and Engineering > School of Electrical Engineering, Electronics and Computer Science
Depositing User: Symplectic Admin
Date Deposited: 28 Apr 2023 08:27
Last Modified: 06 Jul 2023 10:13
DOI: 10.1021/jacsau.3c00087
Open Access URL: https://pubs.acs.org/doi/10.1021/jacsau.3c00087
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URI: https://livrepository.liverpool.ac.uk/id/eprint/3170031