Coupling nitrate capture with ammonia production through bifunctional redox-electrodes

Kwiyong Kim, Alexandra Zagalskaya, Jing Lian Ng, Jaeyoung Hong, Vitaly Alexandrov, Tuan Anh Pham, Xiao Su

Research output: Contribution to journalArticlepeer-review

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.
Original languageEnglish (US)
Article number823
JournalNature communications
Volume14
Issue number1
Early online dateFeb 14 2023
DOIs
StatePublished - Dec 2023

ASJC Scopus subject areas

  • General
  • General Physics and Astronomy
  • General Chemistry
  • General Biochemistry, Genetics and Molecular Biology

Fingerprint

Dive into the research topics of 'Coupling nitrate capture with ammonia production through bifunctional redox-electrodes'. Together they form a unique fingerprint.

Cite this