Coupling nitrate capture with ammonia production through bifunctional redox-electrodes

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

doi:10.1038/s41467-023-36318-1

Title: Coupling nitrate capture with ammonia production through bifunctional redox-electrodes

Journal Article · 13 February 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-36318-1 · OSTI ID:1924560

; Zagalskaya, Alexandra; Ng, Jing Lian;

; Alexandrov, Vitaly; Pham, Tuan Anh;

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.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1924560

Report Number(s):: LLNL--JRNL-855718; 823; PII: 36318

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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