Can we use mine waste as substrate in constructed wetlands to intensify nutrient removal? A critical assessment of key removal mechanisms and long-term environmental risks

•High removal of N and P was simultaneously achieved in mine waste-based wetlands.•Key functional genes and metabolisms of nitrogen cycle are strongly enriched.•Nutrient uptake by plants declined due to the leached heavy metals from mine waste.•Clogging risk in mine waste-based CWs was accelerated due to higher EPS production. The utilization of natural ores and/or mine waste as substrate in constructed wetlands (CWs) to enhance nutrient removal performance has been gaining high popularity recently. However, the knowledge regarding the long-term feasibility and key removal mechanisms, particularly the potential negative environmental effects of contaminants leached from mine waste is far insufficient. This study, for the first time, performed a critical assessment by using different CWs with three mine waste (coal gangue, iron ore and manganese ore) as substrates in a 385-day experiment treating wastewater with varying nutrient loadings. The results showed that the addition of mine waste in CWs increased removal of total phosphorus (TP) by 17-34%, and total nitrogen (TN) by 11-51%. The higher removal of TP is mainly attributed to the strong binding mechanism of phosphate with the oxides and hydroxides of Mn, Fe and/or Al, which are leached out of mine waste. Moreover, integration of mine waste in CWs also significantly stimulated biofilm establishment and enriched the relative abundance of key functional genes related to the nitrogen cycle, supporting the observed high-rate nitrogen removal. However, leaching of heavy metals (Fe, Mn, Cu and Cr) from the beded mine waste in the experimented CWs was monitored, which further influenced cytoplasmic enzymes and created oxidative stress damage to plants, resulting in a decline of nutrient uptake by plants.