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Direct electrosynthesis and separation of ammonia and chlorine from waste streams via a stacked membrane-free electrolyzer

Author

Listed:
  • Jianan Gao

    (New Jersey Institute of Technology)

  • Qingquan Ma

    (New Jersey Institute of Technology)

  • Zhiwei Wang

    (Tongji University)

  • Bruce E. Rittmann

    (Arizona State University)

  • Wen Zhang

    (New Jersey Institute of Technology
    New Jersey Institute of Technology)

Abstract

Electrosynthesis, a viable path to decarbonize the chemical industry, has been harnessed to generate valuable chemicals under ambient conditions. Here, we present a membrane-free flow electrolyzer for paired electrocatalytic upcycling of nitrate (NO3−) and chloride (Cl−) to ammonia (NH3) and chlorine (Cl2) gases by utilizing waste streams as substitutes for traditional electrolytes. The electrolyzer concurrently couples electrosynthesis and gaseous-product separation, which minimizes the undesired redox reaction between NH3 and Cl2 and thus prevents products loss. Using a three-stacked-modules electrolyzer system, we efficiently processed a reverse osmosis retentate waste stream. This yielded high concentrations of (NH4)2SO4 (83.8 mM) and NaClO (243.4 mM) at an electrical cost of 7.1 kWh per kilogram of solid products, while residual NH3/NH4+ (0.3 mM), NO2− (0.2 mM), and Cl2/HClO/ClO− (0.1 mM) pollutants in the waste stream could meet the wastewater discharge regulations for nitrogen- and chlorine-species. This study underscores the value of pairing appropriate half-reactions, utilizing waste streams to replace traditional electrolytes, and merging product synthesis with separation to refine electrosynthesis platforms.

Suggested Citation

  • Jianan Gao & Qingquan Ma & Zhiwei Wang & Bruce E. Rittmann & Wen Zhang, 2024. "Direct electrosynthesis and separation of ammonia and chlorine from waste streams via a stacked membrane-free electrolyzer," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-52830-4
    DOI: 10.1038/s41467-024-52830-4
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    References listed on IDEAS

    as
    1. Lu Lu & Jeremy S. Guest & Catherine A. Peters & Xiuping Zhu & Greg H. Rau & Zhiyong Jason Ren, 2018. "Wastewater treatment for carbon capture and utilization," Nature Sustainability, Nature, vol. 1(12), pages 750-758, December.
    2. Wei Liu & Pengbo Zhai & Aowen Li & Bo Wei & Kunpeng Si & Yi Wei & Xingguo Wang & Guangda Zhu & Qian Chen & Xiaokang Gu & Ruifeng Zhang & Wu Zhou & Yongji Gong, 2022. "Electrochemical CO2 reduction to ethylene by ultrathin CuO nanoplate arrays," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    3. Yong Yuan & Aiwen Lei, 2020. "Is electrosynthesis always green and advantageous compared to traditional methods?," Nature Communications, Nature, vol. 11(1), pages 1-3, December.
    4. Wenhui He & Jian Zhang & Stefan Dieckhöfer & Swapnil Varhade & Ann Cathrin Brix & Anna Lielpetere & Sabine Seisel & João R. C. Junqueira & Wolfgang Schuhmann, 2022. "Splicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    5. Lauren F. Greenlee, 2020. "Recycling fertilizer," Nature Energy, Nature, vol. 5(8), pages 557-558, August.
    6. Mengyan Hou & Long Chen & Zhaowei Guo & Xiaoli Dong & Yonggang Wang & Yongyao Xia, 2018. "A clean and membrane-free chlor-alkali process with decoupled Cl2 and H2/NaOH production," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
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