Anaerobic Ammonium Removal Pathway Driven by the Fe(II)/Fe(III) Cycle through Intermittent Aeration

Feammox, that is, Fe(III) reduction coupled to anaerobic ammonium oxidation, has been reported to play an important role in the nitrogen cycle in natural environments. However, the application of Feammox in wastewater treatment is limited because continuous Fe(III) supplementation is required for achieving continuous nitrogen removal, which is not feasible in practice. In this study, air was aerated intermittently into the Feammox system containing iron and high-content ammonium for oxidizing Fe(II) generated from Feammox to Fe(III), then, the produced Fe(III) participated in the next round of Feammox, leading to continuous nitrogen removal through the Fe(II)/Fe(III) cycle. The results showed that after each 10 min of aeration (150 mL/min), every 6-7 days, dissolved oxygen (DO) increased from 0 to about 0.4 mg/L, accompanied by a decrease in Fe(II) and an increase in Fe(III). One day after the aeration, DO was undetectable, and then, Fe(II) content increased and Fe(III) content decreased. On day 90, NH₄⁺-N content in the aerated reactor was only 10.2 mg/L, while it remained at around 288.3 mg/L in the aeration-free group. X-ray diffraction showed that the generated Fe(III) through air aeration was Fe(OH)₃. Microbial analysis showed that anammox and nitrification/denitrification could be excluded in the system. This NH₄⁺ removal process, driven by the Fe(II)/Fe(III) cycle with O₂ as the terminal electron acceptor, might be used as an in situ remediation method for treating high-content NH₄⁺.