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Per- and polyfluoroalkyl substances (PFAS) in surface and ground waters supplying municipal drinking water are a growing concern. However, PFAS concentrations in water treatment residuals (WTRs)-a solid by-product of water treatment-have yet to be explored. In a first of its kind assessment, we examine PFAS occurrence in seven calcium (Ca)-, iron-, and aluminum-based drinking water treatment residuals (DWTRs) and one wastewater effluent treatment residual (WWETR) produced using aluminum chlorohydrate (ACH). Only perfluoroalkyl acids (PFAAs) were detected, with total PFAA concentrations in the seven DWTRs produced from naturally recharged water sources ranging from 0 to ∼3.3 μg kg -1 ; no PFAS were detected in either of the Ca-DWTRs. The ACH-WWETR contained the highest number and concentration of PFAAs (34 μg kg -1 ). Desorption of resident PFAAs from the WTRs was negligible for the carboxylates (PFCAs). Some desorption of the sulfonates (PFSAs) was detected, particularly for PFOS which had the highest concentration among all resident PFAAs. The ACH-WWETR was further evaluated for its potential to attenuate additional PFAAs (3500 μg mL -1 total PFAAs) in a biosolid-derived porewater matrix. Sorption was highest for long-chain PFAAs and subsequent desorption of the adsorbed PFAAs ranged from 0% to no more than 26%, with the WWETR mass added strongly affecting both PFSA and PFCA sorption/desorption. These findings suggest that WTRs, if introduced into the environment, are unlikely to be a major source of PFAS. Also, the use of particular WTRs as amendments may provide a beneficial reduction in PFAS mobility., (© 2023 The Authors. Journal of Environmental Quality © 2023 American Society of Agronomy, Crop Science Society of America, and Soil Science Society of America.)

Drinking water treatment residuals (DWTRs), solid by-products of drinking water treatment, are dominated by calcium (Ca), iron (Fe), or aluminum (Al), depending on the coagulant used. DWTRs are often landfilled, but current research is exploring options for beneficial reuse. Previous studies have shown that Al- and Fe-rich materials have potential to reduce the mobility of per- and polyfluoroalkyl substances (PFAS). Here, we investigated how amending biosolids with 5% wt/wt DWTRs affected plant bioavailable PFAS in two different simulated scenarios: (1) agricultural scenario with Solanum lycopersicum (tomato) grown in soil amended with an agronomically relevant rate of DWTR-amended biosolids (0.9% w/w, resulting in 0.045% w/w DWTR in the biosolids-amended soil) and (2) mine reclamation scenario examining PFAS uptake by Lolium perenne (perennial ryegrass) grown in soil that received DWTR-amended biosolids amendment at a rate consistent with the mine remediation (13% w/w, resulting in 0.65% w/w DWTR in the biosolids-amended soil). Amending biosolids with Ca-DWTR significantly reduced perfluorobutanoic acid (PFBA) uptake in ryegrass and perfluorohexanoic acid uptake in tomatoes, possibly due to DWTR-induced pH elevation, while Fe-DWTR amendment reduced PFBA bioaccumulation in ryegrass. The Al-DWTR did not induce a significant reduction in accumulated PFAS compared to controls. Although the reasons for this finding are unclear, the relatively low PFAS concentrations in the biosolids and relatively high Al content in the biosolids and soil may be partially responsible., (© 2023 The Authors. Journal of Environmental Quality © 2023 American Society of Agronomy, Crop Science Society of America, and Soil Science Society of America.)

Toxicogenomic responses in Medicago truncatula A17 were monitored following exposure to biosolids-amended soils. Treatments included biosolids produced using a pilot wastewater treatment plant with either no metal introduced into the influent (control); bulk/ionic TiO2, ZnO, and AgNO3 added to influent (bulk/dissolved treatment); or Ag, ZnO, and TiO2 engineered nanomaterials added to influent (ENM treatment) and then added to soil, which was aged in the field for 6 months. In our companion study, we found inhibition of nodulation in the ENM but not in the bulk/dissolved treatment. Gene expression profiling revealed highly distinct profiles with more than 10-fold down-regulation in 239 genes in M. truncatula roots from the ENM treatment, while gene expression patterns were similar between bulk/dissolved and control treatments. In response to ENM exposure, many of the identified biological pathways, gene ontologies, and individual genes are associated with nitrogen metabolism, nodulation, metal homeostasis, and stress responses. Expression levels of nine genes were independently confirmed with qRT-PCR. Exposure to ENMs induced unique shifts in expression profiles and biological pathways compared with bulk/dissolved treatment, despite the lack of difference in bioavailable metal fractions, metal oxidation state, and coordination environment between ENM and bulk/dissolved biosolids. As populations of Sinorhizobium meliloti Rm2011 were similar in bulk/dissolved and ENM treatments, our results suggest that inhibition of nodulation in the ENM treatment was primarily due to phytotoxicity, likely caused by enhanced bioavailability of Zn ions.