Abstract

Nanomaterials present in wastewater can pose a significant threat to aerobic granular sludge (AGS) systems. Herein, we found that compared to graphene nanomaterials (G-NMs), the long-term presence (95 days) of graphene oxide nanomaterials (GO-NMs) resulted in an increased proliferation of filamentous bacteria, poorer sedimentation performance (SVI30 of 74.1mL/g) and smaller average particle size (1224.4µm) of the AGS. In particular, the GO-NMs posed a more significant inhibitory effect to the total nitrogen removal efficiency of AGS (decreased by 14.3%), especially for the denitrification process. The substantial accumulation of GO-NMs within the sludge matrix resulted in a higher level of reactive oxygen species in AGS compared to G-NMs, thereby inducing lactate dehydrogenase release, and enhancing superoxide oxidase and catalase activities. Such excessive oxidative stress could potentially result in a significant reduction in the activity of nitrogen metabolism enzymes (e.g., nitrate reductase and nitrite reductase) and the expression of key functional genes (e.g., nirS and nirK). Altogether, compared to G-NMs, prolonged exposure to GO-NMs had a more significant chronic toxicity effect on AGS systems. These findings implied that the presence of G-NMs and GO-NMs is a hidden danger to biological nitrogen removal and should receive more attention. Environment implicationDue to the diverse applications, graphene and graphene oxide have a high probability of being released into the aquatic ecosystems, potentially polluting to the aquatic environment. Several studies have previously explored the acute toxicity effect of graphene and graphene oxide on biological wastewater treatment systems. However, their chronic toxicity effect on aerobic granular sludge (AGS) systems have not yet been experimentally elucidated. This study implies that the long-term presence of graphene and graphene oxide in AGS systems is a hidden danger to the denitrification process and should receive more attention.

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