Eutrophication control requires cost-effective and sustainable technologies capable of simultaneously removing nitrogen and phosphorus from wastewater treatment plant (WWTP) effluents. Widely used post-treatment systems, treatment wetlands (TWs) typically exhibit limited nutrient removal because of imbalances in electron supply and demand, and rapid saturation of substrate adsorption capacity. In this study, immobile iron-rich particles (IIRPs) were introduced into TWs via a drainage-injection strategy to enhance nutrient removal from municipal WWTP effluent. Following the start-up phase, the IIRP-amended TWs consistently achieved effluent concentrations that met the target quasi-Class IV surface water quality standards (TN ≤ 10 mg L−1; TP ≤ 0.3 mg L−1) for 300 days of continuous operation. The enhanced NH4+-N and TN removal with iron-rich particles amendment could not be attributed to nitrification or anammox, as evidenced using qPCR, metagenomic binning, and removal profiles. Instead, Fe–N redox-coupling processes, including Fe(III) reduction-driven and Fe(II) oxidation-driven nitrogen-removal pathways, contributed to enhanced nitrogen removal. The IIRPs amendment increased the equilibrium phosphorus adsorption capacity of wetland substrate by threefold, and the improved phosphorus retention was attributed to Fe–P interactions. These findings reveal a coupled Fe–N–
P mechanism that enables efficient and stable nutrient removal and provide a mechanistic foundation for developing low-carbon, sustainable strategies to upgrade existing TWs for advanced wastewater polishing.
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