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Controlling the Reaction Pathways of Mixed NOxHy Reactants in Plasma-Electrochemical Ammonia Synthesis
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    Controlling the Reaction Pathways of Mixed NOxHy Reactants in Plasma-Electrochemical Ammonia Synthesis
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 51, 35305–35312
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    https://doi.org/10.1021/jacs.4c12858
    Published December 12, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    Electrochemical activation of dinitrogen (N2) is notoriously challenging, typically yielding very low ammonia (NH3) production rates. In this study, we present a continuous flow plasma-electrochemical reactor system for the direct conversion of nitrogen from air into ammonia. In our system, nitrogen molecules are first converted into a mixture of NOx species in the plasma reactor, which are then fed into an electrochemical reactor. To selectively convert the generated NOx species into NH3, we employed a graph theory approach combined with first-principles calculations to comprehensively enumerate all possible pathways from N2-to-NH3, pinpointing key intermediates (NH2* and NO*). A series of bimetallic catalysts was then designed to target the optimal adsorption and conversion of the limiting intermediate in the NOx-to-NH3 pathway. Using an optimized CuPd foam catalyst, we demonstrated an ammonia production rate of 81.2 mg h–1 cm–2 with stability over 1000 h at an applied current of 2 A.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.4c12858.

    • Materials synthesis and characterization, electrochemical experiments, graph theory methods and DFT simulation, Figures S1–S31, and Tables S1–S3 (PDF)

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    This article is cited by 2 publications.

    1. Lei Xiao, Shiyong Mou, Xiaoyu Lin, Keying Wu, Siyuan Liu, Weidong Dai, Weiping Yang, Chiyao Tang, Chang Long, Fan Dong. Techno-Economic Assessment of Plasma-driven Air Oxidation Coupled with Electroreduction Synthesis of Ammonia. Green Energy & Environment 2025, 360 https://doi.org/10.1016/j.gee.2025.03.009
    2. Kaibin Chu, Bo Weng, Zhaorui Lu, Yang Ding, Wei Zhang, Rui Tan, Yu‐Ming Zheng, Ning Han. Exploration of Multidimensional Structural Optimization and Regulation Mechanisms: Catalysts and Reaction Environments in Electrochemical Ammonia Synthesis. Advanced Science 2025, 12 (11) https://doi.org/10.1002/advs.202416053

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 51, 35305–35312
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.4c12858
    Published December 12, 2024
    Copyright © 2024 American Chemical Society

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