Electrochemically-mediated reactive separation of nitric oxide into nitrate using iron chelate

Abstract

Valorization of nitric oxide is a promising solution for addressing the environmental and resource issues related to the nitrogen cycle. However, low concentrations of nitric oxide combined with impurities in exhaust streams limit its potential, and it requires extensive energy to produce high-purity nitric oxide. Here, we propose a synergistic reactive separation system that combines iron-chelate selective absorption with an electrochemical reaction to convert nitric oxide to nitrate. Among the iron-based chelates tested, EDTA was found to be the most effective in capturing gas-phase nitric oxide. Direct electrochemical oxidation of Fe-EDTA-NO solution exhibited Faradaic efficiency and a partial current density toward nitrate of 70% and 30.1 mA cm^-2 at 2.2 V vs RHE and pH 7, resulting in a 43-fold enhancement of nitrate partial current density and a 2-fold improvement in Faradaic efficiency compared to simple purging without selective absorbent. Nitrate was then selectively recovered from the Fe-EDTA system using simple polarity reversal following electrooxidation with a separation factor of 13 over background sulfate. This study offers a new approach to gas-phase NO remediation and valorization using an electrified means.

Keywords: Absorption; Electrochemical oxidation; Nitrate; Nitric oxides; Reactive separation.