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Coupling nitrate capture with ammonia production through bifunctional redox-electrodes

Author

Listed:
  • Kwiyong Kim

    (University of Illinois Urbana-Champaign
    Ulsan National Institute of Science and Technology (UNIST))

  • Alexandra Zagalskaya

    (Lawrence Livermore National Laboratory
    University of Nebraska-Lincoln)

  • Jing Lian Ng

    (University of Illinois Urbana-Champaign)

  • Jaeyoung Hong

    (University of Illinois Urbana-Champaign
    University of Illinois at Urbana-Champaign)

  • Vitaly Alexandrov

    (University of Nebraska-Lincoln
    University of Nebraska-Lincoln)

  • Tuan Anh Pham

    (Lawrence Livermore National Laboratory
    Lawrence Livermore National Laboratory)

  • Xiao Su

    (University of Illinois Urbana-Champaign)

Abstract

Nitrate is a ubiquitous aqueous pollutant from agricultural and industrial activities. At the same time, conversion of nitrate to ammonia provides an attractive solution for the coupled environmental and energy challenge underlying the nitrogen cycle, by valorizing a pollutant to a carbon-free energy carrier and essential chemical feedstock. Mass transport limitations are a key obstacle to the efficient conversion of nitrate to ammonia from water streams, due to the dilute concentration of nitrate. Here, we develop bifunctional electrodes that couple a nitrate-selective redox-electrosorbent (polyaniline) with an electrocatalyst (cobalt oxide) for nitrate to ammonium conversion. We demonstrate the synergistic reactive separation of nitrate through solely electrochemical control. Electrochemically-reversible nitrate uptake greater than 70 mg/g can be achieved, with electronic structure calculations and spectroscopic measurements providing insight into the underlying role of hydrogen bonding for nitrate selectivity. Using agricultural tile drainage water containing dilute nitrate (0.27 mM), we demonstrate that the bifunctional electrode can achieve a 8-fold up-concentration of nitrate, a 24-fold enhancement of ammonium production rate (108.1 ug h−1 cm−2), and a >10-fold enhancement in energy efficiency when compared to direct electrocatalysis in the dilute stream. Our study provides a generalized strategy for a fully electrified reaction-separation pathway for modular nitrate remediation and ammonia production.

Suggested Citation

  • Kwiyong Kim & Alexandra Zagalskaya & Jing Lian Ng & Jaeyoung Hong & Vitaly Alexandrov & Tuan Anh Pham & Xiao Su, 2023. "Coupling nitrate capture with ammonia production through bifunctional redox-electrodes," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36318-1
    DOI: 10.1038/s41467-023-36318-1
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