# Influence of organic waste amendments on uptake of per and polyfluoroalkyl substances from soil to crops: Insights from long-term field experiments

Toyin Dunsin Saliu, Aurélia Marcelline Michaud, Gabriel Munoz, Quoc Tuc Dinh, Frédéric Feder, Lucile Arrouy, Valérie Sappin-Didier, Françoise Watteau, Sabine Houot, Jinxia Liu, et al.

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## To cite this version:

Toyin Dunsin Saliu, Aurélia Marcelline Michaud, Gabriel Munoz, Quoc Tuc Dinh, Frédéric Feder, et al.. Influence of organic waste amendments on uptake of per and polyfluoroalkyl substances from soil to crops: Insights from long-term field experiments. Science of the Total Environment, 2025, 996, pp.180156. 10.1016/j.scitotenv.2025.180156. hal-05268159

HAL Id: hal-05268159

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Submitted on 19 Sep 2025

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# Influence of organic waste amendments on uptake of per and polyfluoroalkyl substances from soil to crops: Insights from long-term field experiments

Toyin Dunsin Saliu<sup>a</sup>, Aurélia Marcelline Michaud<sup>b</sup>, Gabriel Munoz<sup>a,c</sup>, Quoc Tuc Dinh<sup>a</sup>, Frédéric Feder<sup>d,e</sup>, Lucile Arrouy<sup>a</sup>, Valérie Sappin-Didier<sup>f</sup>, Françoise Watteau<sup>g</sup>, Sabine Houot<sup>h</sup>, Jinxia Liu<sup>i</sup>, Sébastien Sauvé<sup>a,*</sup>

## HIGHLIGHTS

* The Σ75 PFAS in crops from OWP-amended soils remained low <2.5 µg/kg

* Few significant differences observed between crops with and without amendments

* Higher soil organic matter reduces plant uptake of PFAS

* The dominant PFAS in plant samples are PFBA, PFOA and PFOS

* Depending on threshold used, the crops may or may not be safe for human consumption

## GRAPHICAL ABSTRACT

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## ARTICLE INFO

**Keywords:**

Short-chain PFAS

Bioaccumulation

Plant uptake

Biosolids

## ABSTRACT

The use of organic waste products (OWPs) as soil amendments raises concerns due to the potential uptake and accumulation of several environmental contaminants, such as *per*- and polyfluoroalkyl substances (PFAS) in plants. We developed an analytical procedure suitable for screening 75 anionic, zwitterionic, and cationic PFAS in plant tissues (limits of detection: 0.01–0.7 µg/kg). PFAS recoveries were verified in diverse types of crops

<footnote><sup>a</sup> Département de Chimie, Université de Montréal, Montréal, QC H2V 0B3, Canada</footnote>

<footnote><sup>b</sup> INRAE, UMR SAS, Sol Agro et hydrosystème Spatialisation, 35000 Rennes, France</footnote>

<footnote><sup>c</sup> Centre d'expertise en analyse environnementale du Québec, Ministère de l'Environnement, de la Lutte contre les changements climatiques, de la Faune et des Parcs, Québec, QC G1P 3W8, Canada</footnote>

<footnote><sup>d</sup> CIRAD, UPR Recyclage et Risque, F-34398 Montpellier, France</footnote>

<footnote><sup>e</sup> Recyclage et Risque, Univ Montpellier, CIRAD, Montpellier, France</footnote>

<footnote><sup>f</sup> INRAE, ISPA, Bordeaux Sciences Agro, 33140 Villenave d'Ornon, France</footnote>

<footnote><sup>g</sup> INRAE, Laboratoire Sols et Environnement, Université de Lorraine, 54000 Nancy, France</footnote>

<footnote><sup>h</sup> INRAE, UMR ECO SYS, Ecologie fonctionnelle et écotoxicologie des agroécosystèmes, AgroParisTech, Université Paris-Saclay, 78850 Thiverval-Grignon, France</footnote>

<footnote><sup>i</sup> Department of Civil Engineering, McGill University, Montreal, Quebec, H3A 0C3, Canada</footnote>

<footnote>* Corresponding author.
E-mail address: sebastien.sauve@umontreal.ca (S. Sauvé).</footnote>
Composts
Sewage sludge

representative of French agriculture, including maize and wheat (Mainland France) and sugarcane (Overseas France). In the second step, we applied this method to investigate PFAS uptake and accumulation in maize, wheat, and sugarcane grown in experimental fields of France. The Σ75 PFAS in crops harvested from these sites remained relatively low (0.01–2.5 µg/kg) without effects of OWP amendments on plant PFAS concentrations, despite an increase in PFAS in OWP-amended soils. A negative correlation between soil organic carbon and Σ75 PFAS in plants suggests a possible inhibition of PFAS uptake by crops as soil organic matter increases. The dominant PFAS in plant samples included perfluorobutanoic acid (PFBA: 0.10–2.2 µg/kg), perfluorooctanoic acid (PFOA: 0.02–0.66 µg/kg), and perfluorooctane sulfonate (PFOS: 0.01–0.48 µg/kg), accounting for 64–80 % (PFBA), 14–16 % (PFOA) and 6–13 % (PFOS) of the total PFAS, with bioaccumulation factors higher than unity for PFBA and lower than unity for PFOS and PFOA. Bioaccumulation factors were significantly higher in young leaves than in grains, implying limited PFAS transfer to the edible plant tissues of maize and wheat. With the recent lower reference doses (RfD) recommended by the USEPA (2021–2024), the consumption of grains in this study can pose significant risks to humans; however, considering the RfD from EFSA, these crops are safe for human consumption.

# 1. Introduction

The rising cost and the environmental impact of synthetic fertilizers used in agri-food systems have led to a quest for sustainable alternatives. In that respect, soil application of organic waste products (OWP) as an ancestral practice has become a popular substitute for synthetic fertilizers. OWP, such as sewage sludge, biosolids (treated sewage sludge), biowaste composts and digestates, farmyard manure and green waste composts, can improve soil properties by increasing soil organic matter, porosity, stability, water-holding capacity, and fertility (Cooper and DeMarco, 2023; Curci et al., 2020; Adekiya et al., 2020; Lebrazi and Fikri-Benbrahim, 2022; Pizzeghellou et al., 2021; Michaud et al., 2013). Recycling OWPs to agricultural lands also provides environmental benefits and reduces the carbon footprint compared to using landfills and incineration (Michaud et al., 2020).

Nevertheless, the use of these soil amendments raises concerns over their long-term impacts, primarily due to the putative inputs of toxic environmental contaminants and the risks of transfer to soil-plant systems (Lee et al., 2014; Costello and Lee, 2020; Scearce et al., 2023; Adu et al., 2023; He et al., 2024; Habimana and Sauvé, 2025). Recently, per- and polyfluoroalkyl substances (PFAS), a group of manmade organic compounds recognized for their persistence and pervasive prevalence, have come under rigorous scrutiny from the environmental science and health community. PFAS encompass a wide diversity of thousands of organofluorine chemicals listed in more than 200 use categories (Glüge et al., 2020). Though many PFAS exhibit persistent, toxic, and bio-accumulative properties (Brunn et al., 2023), only a few historic compounds are currently regulated. Key PFAS sources to the environment include emissions from fluorochemical manufacturers, the use of aqueous film-forming foams (AFFFs) in fire emergencies (oil fires) or fire equipment testing, and release from personal care products (e.g., cosmetics), waterproof textiles, and waste-receiving facilities (e.g., wastewater treatment plants and landfills) (Glüge et al., 2020; Fredriksson et al., 2022; Høisæter et al., 2019).

PFAS have been investigated in different organic waste products, including biosolids (processed sewage sludge) (Kim Lazcano et al., 2019; Moodie et al., 2021; Munoz et al., 2021; Saliu and Sauvé, 2024), sewage sludge (Fredriksson et al., 2022; Aro et al., 2021; Saliu et al., 2024), commercial composts (Sivaram et al., 2022) and animal manure (Munoz et al., 2021). Link et al. recorded concentrations ranging from 1 to 3200 µg/kg for Σ24 anionic PFAS in biosolids generated from wastewater treatment plants in Michigan, USA, with long-chain perfluoroalkyl sulfonates (e.g., perfluorooctane sulfonate (PFOS) and perfluoroalkyl sulfonamide precursors (e.g., MeFOSAA and EtFOSAA) being the predominant compounds (Link et al., 2024). In another study, a wider breadth of anionic, zwitterionic, and cationic PFAS was investigated in OWP for land application in France (Munoz et al., 2021). A zwitterionic precursor, 6:2 fluorotelomer sulfonamide propyl betaine (6:2 FTAB), was found at similar or higher concentration ranges than PFOS in unsorted municipal solid wastes (Munoz et al., 2021). The study from

France also suggested that farmyard manures had overall far lower PFAS concentrations (average value for Σ160 PFAS: 0.81 µg/kg) compared to many urban-sourced organic waste materials (average value for Σ160 PFAS: 307 µg/kg) (Munoz et al., 2021). Additionally, biowaste sorting strongly decreased PFAS concentration in sorted municipal biowaste, with an average value of 21 µg/kg (Munoz et al., 2021).

PFAS accumulation in soils and uptake by plants following the application of OWPs to the soils have been documented in laboratory-controlled microcosms and field experiments (Costello and Lee, 2020; Sivaram et al., 2023; Ghisi et al., 2019; Navarro et al., 2017a; Krippner et al., 2014). PFAS uptake by plants depends on the molecular structure of the different PFAS (chain length, functional groups and polarity), soil biogeochemical characteristics (organic matter, mineral content, pH, and protein content) and plant species (plant protein and lipids) (Wang et al., 2020; Zhu and Kannan, 2019). For instance, Krippner et al. studied the uptake of perfluoroalkyl carboxylic acids (C4-C10 PFCA) and perfluoroalkyl sulfonates (C4, C6, and C8 PFSA) by maize plants in a laboratory-scale study (Krippner et al., 2014). The concentrations of PFAS in maize straw were inversely correlated with perfluoroalkyl chain length, with short-chain PFBA and PFBS exhibiting the highest concentrations. Other studies have also reported enhanced uptake and translocation of short-chain PFAS in crops (Felizeter et al., 2020; Mayakaduwage et al., 2022; Xu et al., 2022). In a field study, Wen et al. investigated the influence of biosolid application rates on PFAS accumulation in soils. With an application rate ranging from 4.6 to 36 tons/ha, PFAA concentration in the soil increased from 44 to 220 µg/kg. The concentration of 12 PFAS in wheat grown in this biosolid-amended soil across all application rates ranged from 140 to 272 µg/kg (root), 36–178 µg/kg (straws), and 7.3–36 µg/kg (grains) (Wen et al., 2014a). The study concluded that PFAS concentrations in crops significantly increased with increasing biosolid application rates. While field studies reporting the influence of OWP applications to agricultural soils on PFAS accumulation in crops are scarce, a few studies available investigated somewhat higher biosolid application rates, that is usually recommended for agricultural land (Wen et al., 2014a; Blaine et al., 2013).

Research on plant uptake of PFAS has predominantly focused on widely studied anionic compounds, particularly perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS); however, few recent studies have included some of the other emerging polyfluoroalkyl ether PFAS (Qian et al., 2023; Zhang et al., 2021a). Comparatively, the body of literature surrounding novel zwitterionic, cationic, and anionic PFAS, such as those identified at high levels in French biosolids, is exceptionally sparse (Munoz et al., 2021). It remains largely unknown whether these PFAS can bioaccumulate to significant levels in crops. The present study aimed to address this critical knowledge gap by evaluating a breadth of OWP-relevant zwitterionic, cationic, and anionic PFAS in diverse crops grown in the French observatory INRAE-CIRAD SOERE PRO network long-term field experiments, covering different soil types and climatic conditions (Michaud et al., 2013). To the best of our knowledge, this is the first study to comprehensively evaluate the
bioaccumulation of anionic, cationic, and zwitterionic PFAS in crops grown in a long-term experimental field with continuous application of different OWPs obtained from various sources. The inclusion of multiple PFAS classes to understand their behaviour in soil-plant systems, combined with the long-term nature of this study, provides unique insights into the possible environmental and agricultural risks associated with recycling various organic wastes to agricultural soils.

# 2. Materials and methods

## 2.1. Experimental site description

The French observatory INRAE-CIRAD SOERE PRO network consists of long-term field experiments carried out to monitor the effect of OWP application on agro-systems (Michaud et al., 2013; SOERE PRO, 2015). Five experimental sites were included in this observatory, including two historic sites, Couhins - C (Bordeaux, Nouvelle-Aquitaine) and La Bouzule - B (Nancy, Grand-Est), established between 1974 and 1996. At these two historical sites, the application of OWP was stopped in 1993 (Couhins) and 2001 (Bouzule). The three other sites include QualiAgro - QA (Feucherolles, Ile-de-France), PROSpective - PSP (Colmar, Grand-Est) and Réunion - RUN (French Overseas, southwestern Indian Ocean). These sites were established between 1998 and 2013 with a continuous OWP application and agro-system monitoring to date. These experimental sites aim to ascertain the long-term effects of recurring OWP application, notably on soil fertility and the potential contamination of soil with organic and inorganic contaminants. The various types of OWP applied on these sites include municipal sewage sludge (SLU) (applied on C, B, PSP, and RUN site); composts of green wastes and sewage sludge (C-GWS) (applied on B, QA, PSP, and RUN site); composts of municipal biowastes (C-BIOW), i.e., composts of green wastes and the separately collected fermentable fraction of the municipal wastes, (applied on QA and PSP); composts of residual municipal solid wastes (C-MSW), i.e., composts made from the residual fraction of municipal solid wastes after separation from papers and cardboard, glass, and dangerous wastes (applied on B and QA); and farmyard manure of dairy cattle (FYM-DC) (applied on QA and PSP). The organic wastes applied on these sites followed the applicable recommended agronomic application rate, with an average application rate of 5-6 tons/ha dm per year in both PROSpective and Réunion sites (Michaud et al., 2020; Michaud et al., 2021). The maximum sludge application rate was 10 tons/ha dw per year in Couhins. To improve the soil organic matter, an average higher rate of 14 tons/ha dw was applied on the QualiAgro site, representing about 1.5-3 fold larger than usual practices (average recommended amounts) (Michaud et al., 2020). In most cases, when the same type of organic waste product (e.g., SLU or C-GWS) was applied at different field sites, it originated from different sources. Additional mineral nitrogen fertilization was applied at doses between 0 and 200 kg N per hectare to maintain per field-experiment equivalent nitrogen level between treatments. Additionally, the nutrients of soils within some sites amended with OWP were augmented with potassium mineral fertilizer (sites C, B and RUN) and phosphorus mineral fertilizer (at sites B, PSP and RUN) for nutrient balance and optimal plant growth. For each site and treatment year, a control site was selected, receiving the maximal dose of nitrogen mineral fertilization and no OWPs. Similar pesticide treatments and cropping techniques were applied to each plot and treatment in each site and control.

The soil types across the sites were luvisol (Couhins and QualiAgro), calcisol (la Bouzule and PROSpective), and nitisol (RUN), with organic matter varying from 1.8 to 3.6 % (Michaud et al., 2025). The soil pH varied from 5.6 (Couhins) to 6.1 (RUN), 7.1 (QualiAgro), 7.5 (la Bouzule), and 8.4 (PROSpective).

Maize was cultivated at Couhins-C, QualiAgro-QA, and PROSpective-PSP, while wheat and sugarcane were grown at La Bouzule and the RUN site, respectively. Replicated plots with identical application conditions and crop types were established for each treatment.

## 2.2. Crop harvesting and plant sample collection from soere pro network

Plant samples from each replicate plot were harvested, processed, and analyzed separately. The crops from all sites were harvested after reaching maturity, except for the young maize leaves, which were harvested at the 10-12 leaf stage in the Couhins site. A total of 108 historical samples of corn (grains, leaves), wheat and sugarcane from these five sites were collected from 1986 to 2017. For the Couhins site, young-stage maize leaves (when the roots are in the topsoil layer where OWP is mixed with soils) were harvested, while grains were harvested after maturity. From 3 replicate plots, 18 controls and 18 crops harvested from amended soil (maize grains and leaves) were harvested from 1986 to 1998. Maize grains were also harvested in 2012 and 2014 in QualiAgro (6 control and 24 maize grains from amended soil, 3 replicates per treatment). In PROSpective, 24 maize grain samples were harvested from different plots between 2009 and 2017, consisting of 6 control samples and 18 amended samples (3 replicates per treatment). Wheat grains (12 samples) were harvested from La Bouzule at maturity in 1998, consisting of 9 treated samples and three controls, all harvested from 3 plots providing replicates for each treatment applied. Maize and wheat grain samples were dried at 50 °C and then stored in an archival sample bank in darkness and ambient conditions of temperature/humidity. The sugarcane rods harvested from the RUN site with 2 replicates per treatment were washed with MiliQ water, brushed to remove adhering dirt, and washed again. They were then crushed, lyophilized, and finely ground before storage. The selected samples (Table S4) were shipped to the UdeM laboratory, where PFAS analyses were carried out.

A companion study by Michaud et al. (Michaud et al., 2025). reported PFAS concentrations in soil samples collected from the same sites where the crops in the present study were harvested. The study discussed in depth the occurrence of PFAS and Kd partitioning in soil and soil waters, which ascertains PFAS bioavailability through soil pore water or possible leaching to groundwater (Michaud et al., 2025). The soil data from the report will be used in this study only to compute bioaccumulation factors and assist in BAF interpretation.

Using the crop yields recorded from each site (Table S5), the amounts of PFAS taken up by the crops from the soil per hectare were calculated (Eq. 1):

$$PFAS uptake (\mu g/ha) = PFAS conc. in Plant (\mu g/kg) \times plant yields (kg/ha) \quad (1)$$

## 2.3. Standards and reagents

For targeted PFAS analysis, 75 certified native standards were purchased from Wellington Laboratories (Guelph, ON, Canada) (for negative or positive ion mode PFAS) or the Fluobon Surfactant Institute (Beijing, China) (for additional positive ion mode PFAS). Isotopically-labelled PFAS internal standards were also acquired from Wellington Laboratories (Guelph, ON, Canada).

Acetonitrile, methanol, ammonium acetate, ammonium fluoride and HPLC-grade water containing 0.1 % formic acid were purchased from Fisher Scientific (Whitby, ON, Canada). Ammonium acetate (purity ≥98 %) and formic acid (reagent grade, purity ≥95 %) were acquired from Sigma-Aldrich (St. Louis, MO, USA). Supelclean ENVI-Carb cartridges (500 mg/6 mL) were obtained from Supelco (Bellefonte, PA, USA). Further details regarding target analytes, internal standards, reagents, and other materials are presented in the Supporting Information (Table S1).

## 2.4. Sample preparation and extraction

Upon sample reception, the plant samples were ground into powder and homogenized using a methanol-washed mortar and pestle. They were then returned to their original sample jars and stored at -20 °C
until sample extraction. Samples were extracted using previously validated methods by Munoz et al (Munoz et al., 2018). The description of the extraction method is presented in the supplementary file (Section 1.1). All extracts were analyzed using ultra-high-performance liquid chromatography coupled with high-resolution mass spectrometry (Thermo UHPLC-HRMS Orbitrap Q-Exactive) via a polarity-switching electrospray ionization source (Munoz et al., 2021).

## 2.5. Method validation and quality assurance/quality control

Method performance was assessed through recovery, accuracy, and precision tests using representative plant matrices. Absolute recovery was evaluated in grass, while accuracy and precision were verified in winter wheat, sugar cane, and corn. Matrix-based calibration was established using corn samples. Quality control measures included the use of surrogate internal standards, procedural blanks, and correction for background contamination where applicable. Detailed QA/QC protocols and validation results are provided in the Supporting Information (Section S1.2 and Table S3).

## 2.6. Statistical analyses

The statistical analyses in this study were performed using SPSS 23.0 and JMP® (Version 18.1), SAS Institute Inc., Cary, NC, 1989–2023 for Windows software. The Shapiro-Wilk and Kolmogorov-Smirnov tests were applied to investigate the data’s distribution. Log transformation was used to normalize the non-normally distributed data or analyzed using a non-parametric test. Kruskal-Wallis and Mann-Whitney tests were employed to evaluate the significant differences in PFAS concentrations within crops grown on different OWP-amended soil and controls. After testing for data normality and log transformation, a linear regression analysis was conducted to determine the relationships between soil organic carbon, soil pH, and the degree of PFAS bioaccumulation in crops. The results were confirmed with a Pearson test ($p < 0.01$).

## 2.7. Bioaccumulation factor and dietary intake estimation

The bioaccumulation factor (BAF) was computed using Eqs. 2 and 3, which is defined as the ratio of PFAS concentration in plants and PFAS concentration in soil (Liu et al., 2019a). A BAF value >1 means PFAS concentration in plants is greater than in the soil, indicating a significant PFAS bioaccumulation in the plant. In contrast, a BAF value <1 indicates limited uptake or accumulation. Soil data are discussed in-depth in a companion paper focusing on water-soil partitioning of PFAS at SOERE-PRO site (Michaud et al., 2025)

$$ \text{BAF for } \sum_{75} \text{PFAS} = \frac{\text{Concentration of } \sum_{75} \text{PFAS in plants} \left( \frac{\mu g}{kg} \right)}{\text{Concentration of } \sum_{75} \text{PFAS in soil} \left( \frac{\mu g}{kg} \right)} \quad (2) $$

$$ \text{BAF for individual PFAS} = \frac{\text{Concentration of indiv. PFAS in plant} \left( \frac{\mu g}{kg} \right)}{\text{Concentration of indiv. PFAS in soil} \left( \frac{\mu g}{kg} \right)} \quad (3) $$

The consumption of crops grown in OWP-amended soil has been identified as a potential route of human exposure to PFAS. The estimated daily intake (EDI, ng/kg body weight/day) can be used to assess the risk associated with consuming PFAS-contaminated food. The EDI is generally calculated using Eq. 4 (Torres and De-la-Torre, 2023).

$$ \text{EDI} = \frac{\text{DC}*\text{FC}}{\text{BW}} \quad (4) $$

Where DC is the daily grain consumption (g/day), FC is the

concentration of PFAS in grain samples (ng/g), and BW is the body weight (kg). The EDI obtained in this study was then compared with the tolerable daily intake (TDI) reference guidelines, which are determined by national or international authorities (Torres and De-la-Torre, 2023).

On a global scale, maize and wheat grains constitute a vital part of the human diet, consumed in various forms, including corn or wheat flour, cornflakes, bread, tortillas, corn or wheat starch, popcorn, wheat noodles and pasta, wheat cakes, and wheat beverages. (Poutanen et al., 2022)

To calculate the EDI in this study, an average value of 30 g/day of maize grains (children and teenagers aged 7–17 years) and 50 g/day (adults ≥18 years) with an average body weight of 45 kg and 66 kg, respectively taking into consideration the global and the EFSA average daily consumption rates (Statista Research Department, 2024; Erenstein et al., 2022; EFSA, 2024).

Wheat is the second most widely consumed grain after rice, with daily consumption exceeding that of corn. Based on the STATISTA report for European wheat consumption rate (Statista Research Department, 2024; Shahbandeh, 2025), we used the average daily wheat consumption rate of 246 g/day for adults (Statista Research Department, 2024; Shahbandeh, 2025). For the EDI calculation for wheat grains, the daily consumption rate was set at 120 g of wheat for children (presumed to weigh 30 kg) and 260 g of wheat for adults (presumed to weigh 66 kg) (Statista Research Department, 2024; Shahbandeh, 2025).

For risk assessment purposes, the relative risk (RR) was calculated using Eq. 5.

$$ \text{RQ} = \frac{\text{EDI}}{\text{RfD}} \quad (5) $$

Where RQ is the risk quotient, EDI is the estimated daily intake (ng/kg body weight/day), and RfD is the Reference Dose, generally determined by national or international authorities. RfD or tolerable daily intake (TDI) values represent the threshold that should not pose any substantial risk to human health during a lifetime.

The RfD values established by USEPA for PFOA (20 ng/kg bw/day), PFOS (20 ng/kg bw/day) in 2016 (USEPA PFAS RfD, 2016) and the updated values established in 2021 for PFOA (0.002 ng/kg bw/day) and PFOS (0.1 ng/kg bw/day) (RfD, 2022) were compared with the EDI obtained in this study.

The risk quotient (RQ) was calculated using the tolerable daily intake (TDI or RfD) values established by the European Food Safety Authority (EFSA) for PFOA (0.9 ng/kg bw/day) and PFOS (1.9 ng/kg bw/day) in 2018 (EFSA Panel on Contaminants in the Food Chain (CONTAM) et al., 2018). In a recent regulation, an RfD of 0.63 ng/kg bw/day for four PFAS compounds, PFOA, PFNA, PFOS, and PFHxS, was proposed as tolerable daily intake (TDI) (EFSA Panel on Contaminants in the Food Chain (EFSA CONTAM Panel) et al., 2020). Additionally, the 100 ng/L threshold for 20 PFAS established by the EU in their 2020 Directives (Annex III) (Directives, 2020) was converted to a TDI of 4.3 and 2.9 ng/kg bw/day for children (weight 35, water intake 1.5 L) and adults (weight 70 and water intake of 2 L), respectively. These values were included in the RQ evaluations. This value was also used to calculate the RQ in this study. An RQ < 1 can be interpreted as intake levels below the threshold that pose a health risk. This means that consumption or exposure to this level is considered safe and unlikely to cause adverse health effects, as the RQ value approaches zero. Inversely, we should consider that their exposure begins to pose some potential health risks when RQ increases above 1.

# 3. Results and discussion

## 3.1. Rationales for the choice of analytical methods

We reviewed over 20 analysis methods of PFAS in vegetation
samples, including crops (e.g., maize, wheat), fruits (e.g., strawberry), vegetables (e.g., carrot, lettuce), and aquatic plants (Supporting Information Table S2). The number of targeted PFAS typically ranged between 1 and 20, all negative ion mode analytes. While most studies focused on perfluoroalkyl acids, a few recent studies also included precursors such as FOSA and other sulfonamide derivatives, fluoroteller carboxylates and sulfonates, and phosphate esters/diesters. Current-use fluoroalkyl ethers, including GenX (HFPO-DA) and F-53B (X:2 Cl-PFESA), were included for analysis in at least four studies (Chen et al., 2020a; Chen et al., 2020b; Liu et al., 2019b; Zhang et al., 2021b). Most methods involved a freeze-drying pre-treatment step, while the remainder worked with fresh samples. Extraction methods included ion-pairing extraction with methylterbutylether/tetrabutylammonium hydrogen sulfate, ultrasound-assisted extraction with a range of solvents (e.g., dichloromethane/MeOH, ACN/water, MeOH, with or without NH₄OH or NaOH), focused ultrasonication (FUSLE), and digestion in alkaline methanol. Ratios of organic solvent to sample matrix varied between studies (ratio range per cycle: 3–300 mL/g d.w., most between 10 and 20 mL/g d.w.). Most studies involved subsequent cleanup, using SPE (of water-diluted extracts) or graphite (batch or filtration mode, e. g., ENVI-Carb). Analysis typically involved small volume injection (2–20 µL) of extracts to LC-MS/MS, with limits of detection depending on the effective concentration factor (typical LOD range of 0.005–0.5 ng/g dw). As part of method development, we found that either meth- anol or methanol with ammonium hydroxide (e.g., extractant used in USEPA method 1633) were suitable solvents to extract PFAS from freeze-dried biotic tissues (Carrizo et al., 2023). Performing two extraction cycles at a high solvent-to-matrix ratio (~16.7 mL/g) allowed us to comprehensively extract a broad range of PFAS (see also Section 3.2). To circumvent the losses that may otherwise occur during the SPE of aqueous-diluted samples, ENVI-Carb filtration of methanolic extracts was used instead. The list of target PFAS was expanded to include many negative ion mode (e.g., X:Y PFPi) or positive ion mode (e.g., 6:2 FTAB) precursors previously found in French biosolids (Munoz et al., 2021). Unlike most previous studies, we used the high specificity and sensitivity imparted by a Q-Exactive Orbitrap high-resolution mass spectrometer (LC-HRMS).

For soils, previous extraction methods based on methanol or meth-
anol and a weak base were found ineffective in extracting cationic and
zwitterionic PFAS (Mejia-Avendaño et al., 2017). As part of a previous
study, we tested 19 extraction methods for a loam soil contaminated
with PFAS at ppm levels (Munoz et al., 2018). We found that methanol
containing ammonium acetate drastically enhanced the recovery of
difficult-to-extract PFAS, including 6:2 FTAB, and this approach was
therefore retained here. For the same reason stated earlier, the meth-
anolic soil extracts were cleaned by filtering them through ENVI-Carb
cartridges.

**3.2. Analytical method performance**

The absolute recovery in C4 grasses (Graminae spp.) was within an
80–120 % range with an associated RSD <20 %. The accuracy of matrix
spikes was evaluated in 3 additional types of agricultural plants relevant
to this project (winter wheat, sugar cane, and corn). In most cases, ac-
curacy was within 70–130 %, and the relative precision (% RSD based on
triplicate spikes for each crop type) was <20 %. (Table S3).

The matrix-matched calibration curve in corn matrix yielded deter-
mination coefficients (R (Curci et al., 2020)) within 0.9917–0.9999,
compliant with an in-house performance criterion of R² ≥ 0.9900.
Calculated-back concentrations in each calibration level standard
remained within ±20 % except for five specific PFAS (PFPeS, FHxSA,
FOSAA, 8:2 FTSA, and PFHxSAm) at near-LOQ levels (bias within ±30 %).
Method limits of detection (LOD) were within 0.01–0.7 ng/g for
plant samples (Table S3).

**3.3. Site-specific variation in PFAS concentration and dominant pfas profiles in harvested crops**

Fig. 1 presents PFAS concentrations in crops grown on control and OWP-amended soil, highlighting site-specific variations. The concentration for the Σ75 PFAS in maize grains grown on OWP-amended soil varied from 1.4 to 1.96 µg/kg (Couhins), 0.6–2.2 µg/kg (QualiAgro) and 0.2–1.3 µg/kg (PROspective) while Σ75 PFAS in maize grains grown on corresponding control soils which did not receive any OWP from the sites were 0.02–0.04 µg/kg (Couhins), 0.3–2.0 µg/kg (QualiAgro) and 1.1 µg/kg (PROSpective). For wheat grains grown on La Bouzule, the Σ75 PFAS ranged from 0.2 to 0.5 µg/kg (OWP-amended) and 0.5 µg/kg (control soil), while the Σ75 PFAS in sugarcane harvested from the OWP-amended RUN site was < 0.1 µg/kg and 0.4 µg/kg in the control soil. While the Σ75 PFAS in maize grains harvested from the Couhins site varied from 1.4 to 1.96 µg/kg (amended), and 0.02–0.04 µg/kg (control), the Σ75 PFAS in young maize leaves harvested from this same site and plots increased up to 0.4–2.5 µg/kg (amended), and 0.2–1.9 µg/kg (control). This confirms PFAS accumulate more readily in leafy plant parts compared to grains.

Aside from the significant statistical difference noted in maize grains harvested from soil amended with OWP at Couhins compared to the control (*p* < 0.05), no significant differences were found in PFAS concentrations in crops from other OWP-amended sites (QualiAgro, PROspective, Bouzule, and RUN) when compared to their respective control samples.

Generally, the concentration of ∑75PFAS in crops harvested from all OWP-amended soil in this study (0.02–2.9 µg/kg) is much lower compared to those reported in other studies for wheat grains grown on biosolid-amended soils (∑12PFAS = 7.3–36 µg/kg) (Wen et al., 2014b), lettuce (PFOS - 102 µg/kg, PFHxA - 28.0 µg/kg, PFPeA - 27.2 µg/kg, PFBA - 25.5 µg/kg) (Blaine et al., 2013), and pumpkin (ΣdiPAPs - 0.72 ± 0.21 µg/kg to 15.6 ± 2.7 µg/kg, ∑12PFAAs 3.7 ± 0.7 µg/kg to 22.9 ± 16.7 µg/kg) (Lee et al., 2014). This study used realistic and relatively low biosolid amendment rates and the increase reported in other studies could be ascribed to the increased PFAS concentrations in the biosolid amended soils where those crops were grown (Lee et al., 2014; Blaine et al., 2013; Wen et al., 2014b; Blaine et al., 2014a) further arguing that PFAS concentrations in soils amended with OWP is a crucial factor driving PFAS uptake from soils.

Fig. S1 and Table S5 present the distribution and concentrations of the dominant PFAS detected in crops harvested from the different sites, while Table S6 presents descriptive statistics of PFAS superclass concentrations. Among the 75 PFAS analyzed in this study, fifteen were detected in at least one of the plant samples. However, eight PFAS compounds, namely PFBA, PFHxA, PFOA, PFOS, FOSAA, MeFOSAA, PFDoS, and 8:8 PFPi, accounted for the highest proportion of the total PFAS concentration.

Among the superclasses detected, PFCAs predominated in crops
harvested from all sites, except those harvested from SLU-amended soil
in 1986 and 1993 at the Couhins site, where the sulfonamide class was
dominant (Fig. S1; Fig. S2a and b, Table S6). The sulfonamides detected
at the Couhins site were precursor compounds: N-MeFOSAA (found in
SLU-amended soil in 1986 and 1993) and FOSAA (detected in 1998).
The concentration of N-MeFOSAA in crops harvested from SLU-
amended soil varied from 1.3 to 1.4 µg/kg. FOSAA (0.81 µg/kg) was
detected in crops harvested from the control soil in 1998, which can be
attributed to the potential degradation of precursor compounds like N-
EtFOSAA and N-MeFOSAA (Wen et al., 2018) detected in the corre-
sponding soil, and the plowing taking place within the sites might have
contributed to some mixing across sites. Uptake of MeFOSAA from soils
to crops has been previously reported. Xu et al. reported MeFOSAA
contamination in all vegetable samples harvested from a fluoride in-
dustrial park (FIP) in Changshu City, China, with an average concen-
tration of 7 µg/kg (Xu et al., 2024).

The concentration of PFBA in maize grains harvested across the sites
<figure><img src="image_6.png" /><figcaption>**Fig. 1.** Concentration of summed PFAS (Σ75 PFAS, µg/kg) in crops grown on five different sites of the SOERE-PRO network in France, showing the boxplot concentration in crops grown in biosolid-amended soil vs. in control soil without biosolid amendment. The \* symbol denotes statistically significant differences (p < 0.05) while ‘n.s.’ signifies no significant difference.</figcaption></figure>

varied from 0.4 to 1.86 µg/kg (Couhins), 0.3–2.1 µg/kg (QualiAgro), and 0.2–1.1 µg/kg (PROspective) while the concentrations in wheat grain and sugarcane were 0.1–0.5 µg/kg (Bouzule) and 0.37 µg/kg (RUN) respectively (Fig. S1). Across all crops analyzed in this study, PFBA was the dominant PFAS detected, accounting for 62 % (Couhins), 79 % (QualiAgro), 78 % (PROspective), 69 % (Bouzule), and 75 %

(RUN) of the total PFAS detected in the samples (Fig. 2). The concentration of PFBA recorded in this study is comparable to the concentration reported for wheat harvested from a normal agricultural land (1.2 µg/kg) (Yang et al., 2024) and lower than data recorded for wheat grains (342 µg/kg) (Liu et al., 2019a) and 0.5–37.0 µg/kg recorded for maize grains (Liu et al., 2017a) harvested from farms near a FIP. These reports

<figure><img src="image_7.png" /><figcaption>**Fig. 2.** PFAS relative abundance (% of summed PFAS) in crops grown in situ on five different sites of the SOERE-PRO network in France.</figcaption></figure>
also emphasized the predominance of PFBA, contributing 85% and 58% of the total PFAS detected in their studies, respectively (Liu et al., 2019a; Liu et al., 2017a). The dominance of PFBA in crops has been widely documented and attributed to its low molecular weight and low hydrophobicity, which enhances its mobility as it is less adsorbed to the soil's organic carbon (Wang et al., 2020; Xu et al., 2022; Liu et al., 2019a; Bao et al., 2019).

The average concentrations of PFBA in maize leaves (1.7 ± 1.1 µg/kg, n = 6) were higher than in maize grains (0.95 ± 0.55 µg/kg, n = 6). Studies have confirmed that the bioaccumulation of PFAS in leafy plant parts is higher than in grains, attributed to large leaf areas and increased transpiration rates (Xu et al., 2022; Blaine et al., 2014a; Wen et al., 2016). The longer transit distance of PFAS within the plant and the more substantial physiological barriers between the root and grains or seeds have also been linked to the lower PFAS concentration in grains (Xu et al., 2022; Blaine et al., 2014a). Additionally, Xu et al. recorded higher PFAS concentrations in maize leaves than in maize grain, which was attributed to low translocation within plants and the lower protein and fat content in maize grains (Xu et al., 2022).

For maize grains and leaves harvested from the Couhins site, the concentration of PFOA was below the detection limit, while the concentration of PFOS varied from 0.03 to 0.5 µg/kg. This could be attributed to the variation in the concentrations of PFOA (0.012–1.1 µg/kg) and PFOS (0.04–15.3 µg/kg) in the soil from which these crops were harvested. In contrast, the concentration of PFOA in maize grains across QualiAgro and PROspective sites (0.02–0.66 µg/kg) was higher than PFOS (0.01–0.14 µg/kg), even though PFOS was higher than PFOA in the soils (Fig. S1). In a study conducted by Wen et al., the translocation factor (TF) of PFOA was reported to be 1.7–9.9 times that of PFOS (Wen et al., 2016). The lower TF factor recorded for PFOS was suggested to result from the stronger binding of PFOS to plant roots due to higher lipophilicity and larger molecular size compared to PFOA (Blaine et al., 2014a; Wen et al., 2016). PFOA and PFOS contributed between 2.1% and 13% of the total PFAS concentration in maize grains grown on QualiAgro and PROspective sites (Fig. 2). The concentration of PFOA in this study (0.02–0.66 µg/kg) is comparable to the value of 1.07 µg/kg reported for maize grains harvested from normal farmland in China (Yang et al., 2024).

For the sugarcane harvested from RUN, the dominant PFAS detected were PFBA (0.37 µg/kg), PFOS (0.02–0.04 µg/kg) in control and PFHxA (0.06 µg/kg) in amended samples, accounting for 75%, 12.6% and 12.1% of the total PFAS detected in the sugarcane (Fig. 2). The concentration of PFOA recorded in wheat grains in this study ranged from 0.02 to 0.2 µg/kg, while PFOS was not detected in the wheat grains. The recorded value for PFOA in this study is lower than those reported in another study for wheat grain (1.0 ± 0.1 µg/kg) harvested from biosolid-amended soils (Wen et al., 2014a). Although the concentrations of PFOA and PFOS across all samples in this study were generally low, Fig. S2c shows no clear decline in concentration from the earlier years of this field study to the later years despite PFOA and PFOS phase-out in 2002 (UNEP, 2009). This lack of decline in concentration likely reflects

legacy contamination, ongoing transformation of precursors, and the high environmental stability of PFOA and PFOS.

The bioaccumulation factors (BAF) of these dominant PFAS are presented in Table 1. A BAF value >1 means PFAS concentration in the plant is greater than in the soil, indicating a significant PFAS bio-accumulation in the plant. When detected, the BAFs of PFBA across all sites were higher than other PFAS detected, except the higher BAF recorded for MeFOSAA (5.5 ± 4.8) and PFHxA (3.1 ± 3.5) in grains harvested from the Couhins site. In QualiAgro site, the average BAF for the detected compounds in maize grains harvested from amended soils varied from 5.3 ± 3.5 (PFBA), 0.4 ± 0.9 (PFHxA), 0.2 ± 0.4 (PFOA), 0.1 ± 0.2 (PFOS) and 1.5 ± 3.8 (PFDOS). These values are comparable to values recorded for control crops (Table 1), indicating a background PFAS level in the control soil. Consistent with other studies (Wen et al., 2014a; Navarro et al., 2017b), the BAFs of short-chain PFAS reported for PFBA were higher than those of long-chain PFAS. PFBA (C4) had a higher BAF, increasing to 10.9 ± 3.6 in maize leaves and 5.3 ± 3.6 in maize grains, compared to long-chain PFAS (Table 1). This trend could result from the Casparian strip's structure located within the plant root systems, favouring hydrophobic interactions with organic compounds, hence preferentially retaining long-chain PFAS (Arslan and Gamal El-Din, 2021; Wang et al., 2022). In contrast, the short-chain PFAS would travel easily through the Casparian strip to the shoots through the vascular bundle channel. Furthermore, short-chain PFAS exhibit lower soil-water distribution coefficients ($K_d$), resulting in lower sorption to soil constituents such as organic matter, thus enhancing their mobility, bioavailability and a higher translocation rate within the plant (Felizeter et al., 2020; Michaud et al., 2025; Nguyen et al., 2020; Felizeter et al., 2014). The BAF value reported in our study for PFBA in wheat grains was much lower than those reported by Yang et al. (17.7 ± 6.0) for wheat grown on normal agricultural soils (Yang et al., 2024; Felizeter et al., 2014; Felizeter et al., 2020). Additionally, the BAF value obtained for PFOA in wheat grains (0.2 ± 0.2) is comparable to 0.16 ± 0.05 (Wen et al., 2014a) and 0.12 ± 0.10 (Liu et al., 2017b) from other studies, but lower than the reported value of 5.1 ± 2.9 from another study (Yang et al., 2024).

### 3.4. Effect of OWP type and soil properties on PFAS concentrations in harvested crops

The impact of various OWP treatments on PFAS accumulation in maize, wheat, and sugarcane is presented in Fig. 3. For the Couhins site, sewage sludge (SLU) was the only OWP applied on the soil plots. PFAS concentrations in maize harvested from SLU-amended soils in this site varied from 0.7 to 2.5 µg/kg with an average value of 1.5 µg/kg (maize grains and leaves, n = 6), while the concentration in maize harvested from control soils ranged from 0.04 to 2.2 µg/kg with an average of 0.84 µg/kg (n = 6). Despite PFAS concentrations in SLU-amended soils ranging from 10.6 to 20.1 µg/kg (Table 2) reported in the accompanying study by Michaud et al (Michaud et al., 2025), there was no significant difference observed in PFAS concentrations between maize plants

<caption>**Table 1**</caption>

Variations in bioaccumulation factors (BAF) of frequently detected PFAS in plant samples calculated from their individual concentration in soil and in the plants.

<table><thead><tr><th>Site</th><th>Treatment</th><th>Crop Type</th><th>PFBA</th><th>PFHxA</th><th>PFOA</th><th>PFOS</th><th>MeFOSAA</th><th>PFDOS</th><th>FOSAA</th><th>8:8 PFPi</th></tr></thead><tbody><tr><td rowspan="3">Couhins</td><td>Amended</td><td>Grains</td><td>4.4 ± 3.1</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>5.5 ± 4.8</td><td>0.0 ± 0.0</td><td>0.0</td><td>0.0</td></tr><tr><td>Control</td><td></td><td>0.0 ± 0.0</td><td>3.1 ± 4.4</td><td>0.0 ± 0.0</td><td>0.04 ± 0.03</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0</td><td>0.0</td></tr><tr><td>Amended</td><td>Leaves</td><td>10.9 ± 3.6</td><td>0.0 ± 0.00</td><td>0.0 ± 0.0</td><td>0.02 ± 0.01</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0</td><td>0.0</td></tr><tr><td rowspan="3">QualiAgro</td><td>Control</td><td></td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.02 ± 0.03</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>15.4</td><td>0.0</td></tr><tr><td>Amended</td><td>Maize grains</td><td>5.3 ± 3.6</td><td>0.4 ± 0.9</td><td>0.2 ± 0.4</td><td>0.1 ± 0.2</td><td>0.0 ± 0.0</td><td>1.5 ± 3.8</td><td>0.0</td><td>1.4</td></tr><tr><td>Control</td><td></td><td>4.9 ± 4.9</td><td>1.7 ± 1.7</td><td>3.2 ± 2.4</td><td>0.2 ± 0.2</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0</td><td>0.0</td></tr><tr><td rowspan="3">Prospective</td><td>Amended</td><td>Maize grains</td><td>3.4 ± 5.9</td><td>0.3 ± 0.4</td><td>0.0 ± 0.03</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>1.0</td><td>7.3</td></tr><tr><td>Control</td><td></td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0</td><td>0.0</td></tr><tr><td>Amended</td><td>Wheat grains</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.2 ± 0.2</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.9 ± 1.4</td><td>0.0</td><td>10.4</td></tr><tr><td rowspan="3">Bouzule</td><td>Control</td><td></td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0</td><td>0.0</td></tr><tr><td>Amended</td><td>Sugarcane</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.1 ± 0.03</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0</td><td>0.0</td></tr><tr><td>Control</td><td></td><td>0.0 ± 0.0</td><td>0.5 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0</td><td>0.0</td></tr><tr><td>RUN</td><td>Amended</td><td></td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0</td><td>0.0</td></tr><tr><td>Control</td><td></td><td></td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0 ± 0.0</td><td>0.0</td><td>0.0</td></tr></tbody></table>
<figure><img src="image_8.png" /><figcaption>**Fig. 3.** Effect of treatment types on PFAS concentrations in maize, wheat and sugarcane with statistical difference between treatment types. A non-parametric statistical test, the Mann-Whitney *U* test for control and treatment pairs, while the Wilcoxon rank-sum test was used for maize grains and leaves pairs in Couhins. Asterisks (*) indicate a significant difference within each site at *p* < 0.05, while ‘ns’ signifies no significant difference.</figcaption></figure>

<caption>**Table 2**</caption>

PFAS concentrations (µg/kg) in soils (Michaud et al., 2025) and plants with different OWP treatments with corresponding bioaccumulation factors. Treatments: SLU (municipal sewage sludge), C-BIOW (compost of municipal biowastes), C-GWS (compost of green wastes and sewage sludge), C-MSW (compost of residual municipal solid waste), FYM-DC (farmyard manure of dairy cattle).

<table><thead><tr><th>Site</th><th>Treatments</th><th>Range of Σ75 PFAS in soils (µg/kg)</th><th>Range of Σ75 PFAS in plants (µg/kg)</th><th>Range of bioaccumulation Factor for Σ75 PFAS</th></tr></thead><tbody><tr><td rowspan="2">Couhins</td><td>SLU</td><td>10.6–20.1</td><td>0.7–2.5</td><td>0.02–0.12</td></tr><tr><td>Control</td><td>0.57–2.09</td><td>0.04–2.2</td><td>0.2–1.05</td></tr><tr><td rowspan="5">QualiAgro</td><td>C-GWS</td><td>16.7–20.0</td><td>1.3–2.3</td><td>0.07–0.12</td></tr><tr><td>C-BIOW</td><td>1.79–1.98</td><td>1.1–1.2</td><td>0.54–0.61</td></tr><tr><td>C-MSW</td><td>6.50–7.58</td><td>0.6–0.9</td><td>0.05–0.11</td></tr><tr><td>FYM-DC</td><td>0.69–0.82</td><td>0.9–1.3</td><td>1.03–1.59</td></tr><tr><td>Control</td><td>0.32–0.66</td><td>0.5–2.2</td><td>0.91–3.3</td></tr><tr><td rowspan="4">Prospective</td><td>C-GWS</td><td>5.13–5.73</td><td>0.2–0.3</td><td>0.03–0.05</td></tr><tr><td>SLU</td><td>8.98–9.79</td><td>0.3–0.7</td><td>0.02–0.07</td></tr><tr><td>C-BIOW</td><td>1.62–1.78</td><td>0.3–0.8</td><td>0.19–0.45</td></tr><tr><td>Control</td><td>0–1.3</td><td>0.0–1.2</td><td>0.0–0.9</td></tr><tr><td rowspan="4">La Bouzule</td><td>C-GWS</td><td>3.65</td><td>0.2</td><td>0.05</td></tr><tr><td>SLU</td><td>17.26</td><td>0.5</td><td>0.03</td></tr><tr><td>C-MSW</td><td>2.44</td><td>0.5</td><td>0.2</td></tr><tr><td>Control</td><td>0.32</td><td>0.5</td><td>1.7</td></tr><tr><td rowspan="3">Réunion (RUN)</td><td>C-GWS</td><td>5.87</td><td>0.04</td><td>0.01</td></tr><tr><td>SLU</td><td>4.73</td><td>0.01</td><td>0.002</td></tr><tr><td>Control</td><td>3.73</td><td>0.4</td><td>0.11</td></tr></tbody></table>

(maize grain+leaves) grown on sewage sludge-amended soil and control (maize grain+leaves, Fig. 3). In the Couhins site, a statistical difference (*p* < 0.05) was observed between control maize grains and SLU maize grains. Additionally, a significant difference was equally observed in maize grains and leaves grown on control soil (Fig. 3).

The different OWP applied on plots in the QualiAgro site include compost of municipal biowastes (C-BIOW), compost of green wastes and sewage sludge (C-GWS), compost of residual municipal solid waste (C-MSW) and farmyard manure of dairy cattle (FYM-DC). PFAS concentrations in maize grains harvested from soils amended with these OWPs ranged from 1.3 to 2.3 µg/kg (C-GWS), 1.1–1.2 µg/kg (C-BIOW), 0.6–0.9 µg/kg (C-MSW) and 0.9–1.3 µg/kg (FYM-DC) while the concentration in control maize grains varied from 0.5 to 2.2 µg/kg. The BAF across these treatments ranged from 0.05 to 3.3, with the highest BAF recorded in the control maize grains (Table 2). The elevated PFAS concentration of up to 2.3 µg/kg observed in plants harvested from C-GWS-amended soil can be attributed to the elevated PFAS concentrations in the corresponding amended soil, as reported by Michaud et al. (Michaud et al., 2025) (16.7–20.0 µg/kg, Table 2). The pairwise Wilcoxon non-parametric statistical analysis revealed no significant differences between PFAS concentrations in maize grains harvested from soils receiving different OWPs across the sites (QualiAgro and PROspective) and control soils,

Despite an elevated PFAS concentration recorded for the soil amended with SLU in La Bouzule (17.3 µg/kg) (Michaud et al., 2025), there were no significant differences between PFAS concentrations in wheat grains harvested from this soil (0.5 µg/kg) and wheat from the control plots (0.5 µg/kg). PFAS concentrations in wheat grown on SLU,
C-GWS, and C-MSW-amended soils in La Bouzule show no statistically significant differences from the control (Fig. 3). A similar trend was also observed in sugarcane harvested from the RUN site, which received various soil amendments (SLU, C-GWS, and C-BIOW). Besides PFAS concentrations and compound-specific features, soil properties can significantly influence plant PFAS uptake from soils (Blaine et al., 2014a). Due to strong adsorption to soil organic matter, PFAS in soils could be rendered less accessible for plant uptake; hence, increased soil organic carbon would reduce PFAS uptake by plants (Wang et al., 2020). A significant negative correlation between soil organic carbon and BAF ($r = -0.544, p < 0.01$) was observed in this study (Fig. 4a). A comparable trend has been reported for PFAA uptake in lettuce, where an increase in soil organic carbon (from 0.4 % to 2 % and 6 %) resulted in a decreased BAF, presumably due to the higher sorption capacity of the soil (Blaine et al., 2014b). In a field study, Wen et al. evaluated the uptake of 12 PFAAs by wheat grown on biosolid-amended soils. With an increase in SOC contents to 2.76 % through biosolid application, a decrease in BAF of the PFAAs was recorded (Wen et al., 2014a). Several other studies have confirmed that increasing soil organic carbon through the application of organic composts, sewage sludge, or biosolids reduces PFAS uptake by plants (Blaine et al., 2014a; Bizkarguenaga et al., 2016a; Bizkarguenaga et al., 2016b).

PFAS adsorb to soil organic matter through hydrophobic or electrostatic interactions between anionic PFAS and soil cations or ligands, reducing their mobility and bioavailability. The functional group of PFAS can also form hydrogen bonds and van der Waals forces with the functional groups in soil organic matter. Higher organic matter content will yield more binding sites available for PFAS, which leads to more significant adsorption and reduced bioavailability for plant uptake. It is important to note that we have measured soil organic matter only in the topsoil layer. However, the plant's response to soil organic matter reflects conditions throughout the root zone. Since soil organic matter can

vary and is likely to be lower in deeper soil layers, this may weaken the correlation between PFAS in plant tissues and PFAS and soil organic matter concentration on the top layer of the soils. We must also consider that a significant part of plant uptake of PFAS could be taken up the young stage of the plants, when most of the roots are in the plough layer of the soil that has higher soil organic matter content (and more retained PFAS). Long chain PFAS in the plough layer would be mostly adsorbed to organic matter and better protected against degradation whereas shorter chain PFAS are more mobile and more easily leached into lower soil horizons. This vertical distribution of PFAS (and soil organic matter) within soils definitely complicates the interpretation of simple BAF ratios and also highlights that some relationships may hold better at early growth stages of plants where the sampled soil better reflects the root zone explored by the plant than plant tissues from mature plants where the root zone is much larger and not well represented by sampling surface soils.

Although soil pH can affect PFAS speciation in the soil medium, Figs. 4c suggest a negligible relationship between BAF and soil pH. Most PFAS have extremely low pKa values (strong acids) (Mei et al., 2021), which likely explains why changes in soil pH have insignificant effects on their uptake by crops. Nevertheless, soil pH will impact the solubility of dissolved organic matter and hence the mobility of PFAS that would be associated with organic matter (Tavakkoli et al., 2015).

### 3.5. Periodic trend in PFAS accumulation in maize, wheat and sugarcane

Fig. 5 presents the variations in PFAS concentrations in crops across different years in each site. At the Couhins site, the $\sum_{75}$ PFAS concentration in maize grown on amended soils varied from 1.2 to 1.9 µg/kg (1986), 0.7–1.4 µg/kg (1993), and 1.4–2.5 µg/kg (1998). Within these years, average PFAS concentrations in OWP-amended soil were 11 µg/kg (1986), 18 µg/kg (1993), and 21 µg/kg (1998) (Michaud et al., 2025)

<figure><img src="image_9.png" /><figcaption>**Fig. 4.** Pearson's correlation plots between log-transformed data (A) bioaccumulation factor (BAF) versus soil organic carbon (SOC g/kg), (B) BAF versus $\sum_{75}$ (µg/kg) PFAS in soil (µg/kg), (C) BAF versus soil pH, (D) BAF versus $\sum_{75}$ PFAS in plants (µg/kg). ** P < 0.01; *** P < 0.001.</figcaption></figure>
<figure><img src="image_10.png" /><figcaption>**Fig. 5.** Concentration of PFAS in crops grown on different sites per year. A non-parametric statistical test, the Mann-Whitney test was used. Asterisks (*) indicate a significant difference within each site at *p* < 0.05.</figcaption></figure>

(Fig. 5, Table S7). PFAS concentrations recorded for maize grown on control soil varied from 0.04 to 2.2 µg/kg across these years. Statistically, no significant differences were recorded between maize grown on OWP-amended soil and the control soils across the years, except those recorded in 1986 (p < 0.05) in the Couhins site (Fig. 5). Increased PFAS concentrations were recorded in crops harvested from control soils in 1993 and 1998 compared to 1986 (Fig. 5). This could be ascribed to the plowing taking place within this site and possibly transferring some of the contaminants from the treated sites into the control sites as reported in previous studies by Sepulvado et al. and Michaud et al. (Michaud et al., 2025; Sepulvado et al., 2011).

In QualiAgro, Σ75 PFAS concentration in amended soils varied from 0.7 to 6.5 µg/kg (2012) to 0.8–20 µg/kg (2014), while the concentrations in control soils ranged from 0.5 to 1.8 µg/kg across the years as reported by Michaud et al. (Michaud et al., 2025) (Table S7). This indicates PFAS contamination in the soils through OWP application. Due to the increased PFAS concentrations of up to 20 µg/kg in 2014, the Σ75 PFAS concentrations in maize grains grown on this soil increased from 0.6 to 2.2 µg/kg (Fig. 5, Table S7). Several studies have confirmed linear relationships between PFAS concentrations in soils and crops grown on them (Wang et al., 2020; Lechner and Knapp, 2011; Lesmeister et al.,

2021). However, no significant difference was observed between PFAS concentrations in crops grown on amended soil and the control in 2014, but in 2012 (p < 0.05).

At the PROspective site, PFAS concentrations in maize grains harvested from amended soils varied from 0.3 to 0.33 µg/kg (2009) and 0.2–0.8 µg/kg (2017) when the corresponding soil concentrations ranged from 1.6 to 8.9 µg/kg (2009) and 1.8–9.8 µg/kg (2017). There was no statistically significant difference observed between amended and control maize grains harvested in PROspective across the years (Fig. 5, Table S7).

At the La Bouzule and RUN sites, there was no significant difference in PFAS concentration in crops grown on amended soil compared to control soil, despite the increase in PFAS concentrations in soils amended with OWP (Fig. 5, Table S7). This suggests variability in PFAS behaviour and uptake by crops (Lesmeister et al., 2021).

Despite an increase in PFAS concentrations in amended soils recorded at the Couhins site in 1993 (20.8 µg/kg) and the QualiAgro site in 2012 (20.3 µg/kg), as reported by Michaud et al (Michaud et al., 2025), PFAS levels in crops harvested across all sites and the entire study period (1986–2018) remained below 3 µg/kg. The bioaccumulation factors for each crop showed no significant increase, indicating complex dynamics
of plant uptake over time.

Generally, in the early years of cultivation, PFAS concentrations in the control soils were relatively low compared to those in the later years, which could be attributed to plowing within the plots. Plowing mixes the soil layers over several tens of centimetres and can, therefore, dilute the concentrations in the most superficial layer. The correlation between plant tissue and superficial soil could be disconnected from the actual system if the plant roots are exploring a much deeper range of the soil and the soil-plant comparison is limited to the soil surface. This is an inherent limitation of plant uptake from soil in the case of mature plants extracting a large soil mass that is nearly impossible to fully characterize.

### 3.6. Dietary intake estimation

The EDI data of the PFAS compounds detected in this study across all sites and treatments are presented in Table 3. For maize grains, the EDI obtained for the $\Sigma_{75}$ PFAS ranged from 0.02 to 1.83 ng/kg bw/day calculated for children and 0.02–1.66 ng/kg bw/day. EDI for the $\Sigma_{75}$ PFAS in wheat grains ranged from 0.88 to 11.20 ng/kg bw/day (children) and 0.87–11.03 (adults). These values were lower than the previous EDI recorded for $\Sigma_{12}$ PFAS (11.5–19.5 ng/kg·bw/day) in maize and wheat harvested from farms 10 km from a FIP (Liu et al., 2019a).

The PFAS with the highest EDI in this study was PFBA at 0.21–1.77 ng/kg bw/day (children) and 0.19–1.61 ng/kg bw/day (adults) in maize, while the EDI value in wheat grains ranged from 0.40 to 1.80 ng/kg bw/day (children) and 0.39–1.77 ng/kg bw/day (adults). These values are comparable to the EDI obtained for PFBA in wheat harvested from normal farmland (1.26 ng/kg bw/day) (Yang et al., 2024).

The maximum EDI obtained for PFOA and PFOS for children was 0.55 ng/kg bw/day and 0.12 ng/kg bw/day, respectively, while 0.5 ng/kg bw/day and 0.11 ng/kg bw/day were recorded for adults in maize grains (Table 3). PFOS was not detected in wheat; however, the highest EDI recorded for PFOA were 0.68 ng/kg bw/day (children) and 0.67 ng/kg bw/day for adults (Table 3). These are higher than values obtained for PFOA and PFOS (0.38 ng/kg bw/day) in another study (Yang et al., 2024) but much lower than USEPA-derived oral non-cancer reference doses (RfDs) of 20 ng/kg/day for both PFOS and PFOA established in 2016 (USEPA PFAS RfD, 2016). In 2021, a lower chronic RfD dose of 0.002 ng/kg/day (PFOA) and 0.01 ng/kg/day (PFOS) was established by the USEPA based on human epidemiology studies for developmental/growth effects, cardiovascular health risks, and effects on immune

<table><caption>**Table 3**
The estimated daily intake (EDI) values PFAS in maize and wheat grains (ng/kg bw/day).</caption><thead><tr><th rowspan="2">Maize</th><th rowspan="2">EDI</th><th colspan="2">Children</th><th colspan="2">Adults</th></tr><tr><th>Minimum<br>(ng/kg bw/<br>day)</th><th>Maximum<br>(ng/kg bw/<br>day)</th><th>Minimum<br>(ng/kg bw/<br>day)</th><th>Maximum<br>(ng/kg bw/<br>day)</th></tr></thead><tbody><tr><td rowspan="10">Wheat</td><td>$\Sigma_{75}$<br>PFAS</td><td>0.02</td><td>1.83</td><td>0.02</td><td>1.66</td></tr><tr><td>$\Sigma_{4}$<br>PFAS*</td><td>0.05</td><td>0.71</td><td>0.05</td><td>0.65</td></tr><tr><td>PFBA</td><td>0.21</td><td>1.77</td><td>0.19</td><td>1.61</td></tr><tr><td>PFOA</td><td>0.02</td><td>0.55</td><td>0.02</td><td>0.50</td></tr><tr><td>PFOS</td><td>0.03</td><td>0.12</td><td>0.02</td><td>0.11</td></tr><tr><td>$\Sigma_{75}$<br>PFAS</td><td>0.88</td><td>11.20</td><td>0.87</td><td>11.03</td></tr><tr><td>$\Sigma_{4}$<br>PFAS*</td><td>0.08</td><td>0.68</td><td>0.08</td><td>0.67</td></tr><tr><td>PFBA</td><td>0.40</td><td>1.80</td><td>0.39</td><td>1.77</td></tr><tr><td>PFOA</td><td>0.08</td><td>0.68</td><td>0.08</td><td>0.67</td></tr><tr><td>PFOS</td><td>NA</td><td>NA</td><td>NA</td><td>NA</td></tr></tbody></table>

health. In the present study, the EDI for PFOA and PFOS recorded in maize and wheat at maximum concentration were much higher (0.1 to 0.69 ng/kg bw/day - see Table 3) than the new USEPA chronic RfD values (RfD, 2022). The EDI for PFOA and PFOS across all the OWPs applied were similar and lower than the EFSA standards even at maximum concentration (Table S9).

Considering the new 4 ng/L benchmark adopted for drinking water by the USEPA (RfD, 2022; USEPA, 2024), the RfD calculated from this value was 0.1 ng/kg bw/day (PFOA and PFOS) for an adult of 70 kg and 0.3 ng/kg bw/day for children drinking 2 L of water per day. At maximum PFOA and PFOS concentration in the grains, the EDI recorded values were also higher than the USEPA drinking water PFAS benchmark.

Higher than the RfD established by USEPA in 2021 and 2024, the European Food Safety Authority (EFSA) recommendations for PFOA and PFOS in 2018 were set at 0.9 ng/kg bw/day and 1.9 ng/kg bw/day, respectively (EFSA Panel on Contaminants in the Food Chain (CONTAM) et al., 2018). In a recent regulation, a lower RfD value of 0.63 ng/kg bw/day for four PFAS compounds, PFOA, PFNA, PFOS, and PFHxS, was proposed (EFSA Panel on Contaminants in the Food Chain (EFSA CONTAM Panel) et al., 2020). The EDI recorded for PFOA and PFOS in our study for maize and wheat grains harvested from OWP-amended soil were below EFSA's recommended values for PFOA and PFOS. However, for the $\Sigma_{4}$ EFSA PFAS (PFOA, PFNA, PFOS, and PFHxS), the EDI were slightly higher at maximum concentrations (0.05–0.71 ng/kg bw/day) than the EFSA reference dose (0.63 ng/kg bw/day). With the recent lower RfD recommended by the USEPA (2021–2024), the consumption of grains in this study can pose significant risks to humans; however, considering the higher values of RfD from EFSA, these crops are safe for human consumption.

The influence of treatment types on PFAS EDI in maize and wheat grains is presented in Table S9. Regardless of the treatment type, the EDI for the $\Sigma_{75}$ PFAS, $\Sigma_{4}$ EFSA PFAS, PFOA and PFOS in maize grains were lower than the established tolerable intake by EFSA. In wheat grains, the EDI recorded were also less than the established tolerable daily intake (TDI); however, the EDI for the $\Sigma_{4}$ EFSA PFAS (children: 0.8–1.9 ng/kg bw/day, adults: 0.7–1.7 ng/kg bw/day) were higher than the established TDI by EFSA (0.63 ng/kg bw/day for the sum of PFOA, PFNA, PFOS, and PFHxS), irrespective of the treatment type including the control.

Generally, higher EDI values were recorded for children compared to adults due to a higher food consumption rate per body weight. This confirms that children's exposure to PFAS contamination through food is higher than that of adults, a trend that has been reported earlier (Liu et al., 2019a; Zhang et al., 2017; Klenow et al., 2013). The higher EDI recorded for wheat grains is due to the higher consumption rate of 260 g/day in adults and 120 g/day in children compared to maize, which is 50 g/day in adults.

The relative risk (RQ) was calculated using the TDI values proposed by the EFSA for PFOA (0.9 ng/kg bw/day), PFOS (1.9 ng/kg bw/day) (EFSA Panel on Contaminants in the Food Chain (CONTAM) et al., 2018) and the recent regulation of 0.63 ng/kg bw/day for the sum of PFOA, PFNA, PFOS, and PFHxS (EFSA Panel on Contaminants in the Food Chain (EFSA CONTAM Panel) et al., 2020). The RQ for PFOA (0.01–0.8) and PFOS (0.01–0.06) were less than 1, thus suggesting no significant risks. However, with the lower TDI of 0.63 ng/kg bw/day proposed by the EFSA, the RQ calculated for the $\Sigma_{4}$ PFAS exceeded 1 at maximum concentration, ranging from 0.07 to 1.1 for maize and 0.1–1.1 for wheat, while those calculated for PFOA were below the proposed values (Fig. 6). Using the European Union threshold of 100 ng/L for $\Sigma_{20}$ PFAS in for drinking water, the TDI calculated from this value was used to estimate the RQ values for maize and wheat. The RQ for the $\Sigma_{EU20}$ PFAS in maize were below 1 (children: 0.004–0.4; adult: 0.01–0.5), however, the RQ exceeded 1 in wheat due to higher consumption rate.

Fig. 7 further provides insight into the influence of OWP type on the

<footnote>* $\Sigma_{4}$PFAS: EFSA proposed a tolerable daily intake (TDI) value of 0.63 ng/kg bw/day for the sum of PFOA, PFNA, PFOS, and PFHxS (EDI: estimated daily intake).</footnote>
<figure><img src="image_11.png" /><figcaption>**Fig. 6.** Risk Quotient (RQ) values of PFAS in maize and wheat grains. RQ values were calculated using the TDI established by EFSA for PFOA (0.9 ng/kg bw/day), PFOS (1.9 ng/kg bw/day) and the recent regulation of 0.63 ng/kg bw/day for the ΣEFSA₄ PFAS. RQ for EU₂₀ PFAS was estimated using the 100 ng/L established for drinking water.</figcaption></figure>

<figure><img src="image_12.png" /><figcaption>**Fig. 7.** Influence of treatment types on the risk quotient value estimated for Σ4 EFSA PFAS (PFOA, PFOS, PFNA and PFHxS) in maize and wheat grains. Kruskal-Wallis statistical test shows no significant difference across treatments and control. Risk assessment: CN=FYM = C-BIOW=C-MSW=C-GWS=SLU) for each crop. Treatments: SLU (municipal sewage sludge), C-BIOW (compost of municipal biowastes), C-GWS (compost of green wastes and sewage sludge), C-MSW (compost of residual municipal solid wastes), FYM-DC (farmyard manure of dairy cattle).</figcaption></figure>

RQ values. The RQ values for the Σ₄ EFSA-regulated PFAS were <1 in maize grains but >1 in wheat grains, irrespective of the type of OWPs applied. The Kruskal-Wallis statistical test shows no significant

difference across each treatment, including the control, confirming equal risks across treatment and control. The increase in RQ observed in wheat was primarily driven by the high consumption rate of wheat and
the lower TDI established by EFSA, rather than the specific OWP applied. Even when crops are grown in control soils receiving mineral fertilization, the same increase in EDI is observed. This suggests potential concern for human health under stricter regulatory thresholds. Therefore, it is essential to align risk assessment with appropriate TDI guidelines to ensure a comprehensive evaluation of PFAS exposure risks through dietary pathways.

## 4. Conclusions

This study validated an analytical method suitable for screening a broader range of PFAS in crop samples at ultra-trace levels, achieving analyte recoveries typically ranging from 70 % to 130 %. Despite the high PFAS levels observed in some municipal biosolids and the increase in PFAS concentrations in OWP-amended soil, PFAS concentrations in crops harvested from these sites were relatively low, ranging from 0.03 to 2.5 µg/kg across all sites and treatments. Among the 75 PFAS analyzed in this study, PFBA was responsible for the majority of the summed PFAS, accounting for ~60–80 % of the total PFAS detected in crops. The detection rates of PFOS and PFOA were also high in the crops. PFAS profiles from the historical site Couhins (Nouvelle-Aquitaine) differed from those of others in that the ECF-based precursor NMeFO-SAA was occasionally found in maize crops.

When compared with the EFSA's RfD doses, the EDI for PFOA and PFOS in maize and wheat grains were at a relatively safe level. However, the EDI for the $\sum_{4}^{4}$ EFSA-regulated PFAS in this study was slightly higher than the EFSA RfD for the sum of those four PFAS. This suggests potential concerns for human health through the consumption of maize and wheat grains grown in soils amended with the studied organic waste products and control soils, even though we observed no statistical differences between the control and amended treatments. This should nevertheless be reassessed as dietary reference doses for food are likely to be further adjusted. EFSA is currently using the sum of PFOA, PFNA, PFOS and PFHxS and it must be emphasized that reference dose might need to be updated to integrate a larger number of PFAS – especially the PFAS that are taken up by plants such as PFBA, PFHxA, PFDOs, MeFO-SAA (see Fig. 2). Despite the minimal risks of plant uptake of PFAS observed in this study, applying OWP sourced from wastewater treatment plants receiving industrial or municipal wastewater contaminated with PFAS may, however, result in PFAS transfer to soil and groundwater. Therefore, it remains essential to monitor PFAS levels in OWP before they are land-applied. A key limitation affecting the consistency of comparisons among crops from different treatments in this study is the variability in treatment periods and different OWP sources. However, the archived nature of the dataset provided a unique opportunity to assess PFAS accumulation under real-life field conditions, offering insight into the historical use of legacy PFAS.

### CRediT authorship contribution statement

**Toyin Dunsin Saliu:** Writing – original draft, Visualization, Methodology, Investigation, Formal analysis, Data curation.
**Aurélia Marcelline Michaud:** Writing – review & editing, Visualization, Validation, Supervision, Project administration, Methodology, Investigation, Funding acquisition, Formal analysis, Data curation, Conceptualization.
**Gabriel Munoz:** Writing – review & editing, Validation, Methodology, Formal analysis.
**Quoc Tuc Dinh:** Writing – review & editing, Validation, Methodology, Formal analysis.
**Frédéric Feder:** Writing – review & editing, Methodology, Investigation.
**Lucile Arrouy:** Writing – review & editing, Investigation, Formal analysis.
**Valérie Sappin-Didier:** Writing – review & editing, Supervision, Project administration, Methodology, Investigation, Data curation, Conceptualization.
**Françoise Watteau:** Writing – review & editing, Project administration, Investigation, Formal analysis, Conceptualization.
**Sabine Houot:** Writing – review & editing, Validation, Project administration, Investigation.
**Jinxia Liu:** Writing – review & editing, Validation, Project administration,

Methodology, Funding acquisition, Formal analysis. Sébastien Sauvé: Writing – review & editing, Validation, Supervision, Project administration, Methodology, Investigation, Funding acquisition, Formal analysis, Conceptualization.

### Declaration of competing interest

The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: SÉBASTIEN SAUVÉ reports financial support was provided by Natural Sciences and Engineering Research Council of Canada. SÉBASTIEN SAUVÉ reports financial support was provided by Quebec Research Fund (https://doi.org/10.69777/355389). SÉBASTIEN SAUVÉ reports financial support was provided by Strategic Environmental Research and Development Program. Sébastien Sauvé reports a relationship with Collective Action Law Firm that includes: consulting or advisory. If there are other authors, they declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

### Acknowledgments

The field experiments are part of the SOERE-PRO (network of long-term experiments dedicated to the study of impacts of organic waste product recycling), integrated as a service of the infrastructure "Investment for the future" AnaEE-France, overseen by the French National Research Agency (ANR 11- INBS-0001). We thank all those who participated in the management of the SOERE-PRO sites, especially D. Montenach and C. Resseguier, as well as the partners, notably the Mixed Syndicate Union for Agricultural Recycling Haut-Rhin (SMRA 68), Veolia Research and Innovation (VERI) and Veolia Water. The authors also thank the Natural Sciences and Engineering Research Council of Canada (STPGP 478774), the Fonds Québécois de la Recherche sur la Nature et les Technologies (2015-PR-183278 and https://doi.org/10.69777/355389), and the Canadian Foundation for Innovation (30044) for their financial support. We acknowledge funding by the Strategic Environmental Research and Development Program (SERDP ER19-1157).

## Appendix A. Supplementary data

Supplementary data to this article can be found online at https://doi.org/10.1016/j.scitotenv.2025.180156.

### Data availability

Most of the pertinent data have been included in the supplementary information files. Other data can be requested from the corresponding author.

### References

* Adekiya, A.O., Ejue, W.S., Oleyanju, A., Dunsin, O., Aboyeji, C.M., Aremu, C., Adegbite, K., Akinpelu, O., 2020. Different organic manure sources and NPK fertilizer on soil chemical properties, growth, yield and quality of okra. Sci. Rep. 10 (1), 16083. https://doi.org/10.1038/s41598-020-73291-x

* Adu, O., Ma, X., Sharma, V.K., 2023. Bioavailability, Phytotoxicity and Plant Uptake of per-and Polyfluoroalkyl Substances (PFAS): A Review. J. Hazard. Mater. 447, 130805. https://doi.org/10.1016/j.jhazmat.2023.130805

* Aro, R., Eriksson, U., Kärrman, A., Chen, F., Wang, T., Yeung, L.W.Y., 2021. Fluorine Mass Balance Analysis of Effluent and Sludge from Nordic Countries. ACS EST Water 1 (9), 2087–2096. https://doi.org/10.1021/acsestwater.1c00168

* Arslan, M., Gamal El-Din, M., 2021. Removal of Per- and Poly-Fluoroalkyl Substances (PFASs) by Wetlands: Prospects on Plants, Microbes and the Interplay. Sci. Total Environ. 800, 149570. https://doi.org/10.1016/j.scitotenv.2021.149570

* Bao, J., Yu, W.-J., Liu, Y., Wang, X., Jin, Y.-H., Dong, G.-H., 2019. Perfluoroalkyl Substances in Groundwater and Home-Produced Vegetables and Eggs around a Fluorochemical Industrial Park in China. Ecotoxicol. Environ. Saf. 171, 199–205. https://doi.org/10.1016/j.ecoenv.2018.12.086
Bizkarguenaga, E., Zabaleta, I., Mijangos, L., Iparraguirre, A., Fernández, L., Prieto, A., Zuloaga, O., 2016a. Uptake of Perfluorooctanoic Acid, Perfluorooctane Sulfonate and Perfluoroocytane Sulfonamide by Carrot and Lettuce from Compost Amended Soil. Sci. Total Environ. 571, 444–451. https://doi.org/10.1016/j.scitotenv.2016.07.010.

Bizkarguenaga, E., Zabaleta, I., Prieto, A., Fernández, L.A., Zuloaga, O., 2016b. Uptake of 8:2 Perfluoroalkyl Phosphate Diester and Its Degradation Products by Carrot and Lettuce from Compost-Amended Soil. Chemosphere 152, 309–317. https://doi.org/10.1016/j.chemosphere.2016.02.130.

Blaine, A.C., Rich, C.D., Hundal, L.S., Lau, C., Mills, M.A., Harris, K.M., Higgins, C.P., 2013. Uptake of Perfluoroalkyl Acids into Edible Crops via Land Applied Biosolids: Field and Greenhouse Studies. Environ. Sci. Technol. 47 (24), 14062–14069. https://doi.org/10.1021/es403094q.

Blaine, A.C., Rich, C.D., Sedlacko, E.M., Hundal, L.S., Kumar, K., Lau, C., Mills, M.A., Harris, K.M., Higgins, C.P., 2014a. Perfluoroalkyl Acid Distribution in Various Plant Compartments of Edible Crops Grown in Biosolids-Amended Soils. Environ. Sci. Technol. 48 (14), 7858–7865. https://doi.org/10.1021/es500016s.

Blaine, A.C., Rich, C.D., Sedlacko, E.M., Hyland, K.C., Stushnoff, C., Dickenson, E.R.V., Higgins, C.P., 2014b. Perfluoroalkyl Acid Uptake in Lettuce (*Lactuca Sativa*) and Strawberry (*Fragaria Ananassa*) Irrigated with Reclaimed Water. Environ. Sci. Technol. 48 (24), 14361–14368. https://doi.org/10.1021/es504150h.

Brunn, H., Arnold, G., Körner, W., Rippen, G.K., Steinhäuser, K., Valentín, I., 2023. PFAS: forever chemicals—persistent, bioaccumulative and mobile. Reviewing the status and the need for their phase out and remediation of contaminated sites. Environ. Sci. Eur. 35 (1), 20. https://doi.org/10.1186/s12302-023-00721-8.

Carrizo, J.C., Munoz, G., Vo Duy, S., Liu, M., Houde, M., Amé, M.V., Liu, J., Sauvé, S., 2023. PFAS in Fish from AFFF-Impacted Environments: Analytical Method Development and Field Application at a Canadian International Civilian Airport. Sci. Total Environ. 879, 163103. https://doi.org/10.1016/j.scitotenv.2023.163103.

Chen, C.-H., Yang, S.-H., Liu, Y., Jamieson, P., Shan, L., Chu, K.-H., 2020b. Accumulation and Phytotoxicity of Perfluorooctanoic Acid and 2,3,3,3-Tetrafluoro-2-(Heptafluoropropoxy)Propanoate in Arabidopsis Thaliana and Nicotiana Benthamiana. Environ. Pollut. 259, 113817. https://doi.org/10.1016/j.envpol.2019.113817.

Chen, L., Dai, Y., Zhou, C., Huang, X., Wang, S., Yu, H., Liu, Y., Morel, J.L., Lin, Q., Qiu, R., 2020a. Robust Matrix Effect-Free Method for Simultaneous Determination of Legacy and Emerging Per- and Polyfluoroalkyl Substances in Crop and Soil Matrices. J. Agric. Food Chem. 68 (30), 8026–8039. https://doi.org/10.1021/acs.jafc.0c02630.

Cooper, A., DeMarco, J., 2023. Composted biosolids amendments for enhanced soil organic carbon and water storage in perennial pastures in Colorado. Agric. Ecosyst. Environ. 347, 108401. https://doi.org/10.1016/j.agec.2023.108401.

Costello, M., Liu, L.S., 2020. Sources, fate, and plant uptake in agricultural systems of per- and polyfluoroalkyl substances. Curr. Pollut. Rep. 1–21. https://doi.org/10.1007/s40726-020-00168-y.

Curci, M., Lavecchia, A., Cucci, G., Lacolla, G., De Corato, U., Crecchio, C., 2020. Short-Term Effects of Sewage Sludge Compost Amendment on Semiarid Soil. Soil Syst. 4 (3), 48. https://doi.org/10.3390/soilsystems4030048.

Dirctives, E.U., 2020. The Maximum Concentrations for PFAS Total and Sum of PFAS Are Listed in Part B of Annex I. https://eur-lex.europa.eu/legal-content/EN/TXT/PDF/?uri=CELEX:32020L2184&from=EN.

EFSA, 2024. Food Consumption Statistics for FoodEx2: Level 1 (e.g. Grains and Grain-Based Products). https://www.efsa.europa.eu/en/microstrategy/foodex2-level-1. (Accessed 20 January 2025).

EFSA Panel on Contaminants in the Food Chain (CONTAM), Knutsen, H.K., Alexander, J., Barregård, L., Bignami, M., Brüschweiler, B., Ceccatelli, S., Cottrill, B., Dinovi, M., Edler, L., Grasl-Kraupp, B., Hogstrand, C., Hoogenboom, L. (Ron), Nebbia, C.S., Oswald, I.P., Petersen, A., Rose, M., Roudot, A., Vlemminckx, C., Vollmer, G., Wallace, H., Bodin, L., Cravedi, J., Halldorsson, T.I., Haug, L.S., Johansson, N., van Loveren, H., Gergelova, P., Mackay, K., Levorato, S., van Manen, M., Schwerdtle, T., 2018. Risk to human health related to the presence of perfluorooctane sulfonic acid and perfluorooctanoic acid in food. EFS2 16 (12). https://doi.org/10.2903/j.efsa.2018.5194.

EFSA Panel on Contaminants in the Food Chain (EFSA CONTAM Panel), Schrenk, D., Bignami, M., Bodin, L., Chipman, J.K., del Mazo, J., Grasl-Kraupp, B., Hogstrand, C., Hoogenboom, L. (Ron), Leblanc, J., Nebbia, C.S., Nielsen, E., Ntzani, E., Petersen, A., Sand, S., Vlemminckx, C., Wallace, H., Barregård, L., Ceccatelli, S., Cravedi, J., Halldorsson, T.I., Haug, L.S., Johansson, N., Knutsen, H.K., Rose, M., Roudot, A., Van Loveren, H., Vollmer, G., Mackay, K., Riolo, F., Schwerdtle, T., 2020. Risk to human health related to the presence of perfluoroalkyl substances in food. EFS2 18 (9). https://doi.org/10.2903/j.efsa.2020.6223.

Erenstein, O., Jaleta, M., Sonder, K., Mottaleb, K., Prasanna, B.M., 2022. Global Maize Production, Consumption and Trade: Trends and R&D Implications. Food Sec. 14 (5), 1295–1319. https://doi.org/10.1007/s12571-022-01288-7.

Felizeter, S., McLachlan, M., Voogt, P. de, 2014. Root uptake and translocation of perfluorinated alkyl acids by three hydroponically grown crops. J. Agric. Food Chem. 3334–3342. https://doi.org/10.1021/jf500674j, 6215.

Felizeter, S., Jürling, H., Kotthoff, M., Voogt, P. de, McLachlan, M., 2020. Influence of soil on the uptake of perfluoroalkyl acids by lettuce: a comparison between a hydroponic study and a field study. Chemosphere 260, 127608. https://doi.org/10.1016/j.chemosphere.2020.127608.

Fredriksson, F., Eriksson, U., Kärrman, A., Yeung, L.W.Y., 2022. Per- and Polyfluoroalkyl Substances (PFAS) in Sludge from Wastewater Treatment Plants in Sweden — First Findings of Novel Fluorinated Copolymers in Europe Including Temporal Analysis. Sci. Total Environ. 846, 157406. https://doi.org/10.1016/j.scitotenv.2022.157406.

Ghisi, R., Vamerali, T., Manzetti, S., 2019. Accumulation of Perfluorinated Alkyl Substances (PFAS) in Agricultural Plants: A Review. Environ. Res. 169, 326–341. https://doi.org/10.1016/j.envres.2018.10.023.

Glüge, J., Scheringer, M., Cousins, I.T., DeWitt, J.C., Goldenman, G., Herzke, D., Lohmann, R., Ng, C.A., Trier, X., Wang, Z., 2020. An Overview of the Uses of Per- and Polyfluoroalkyl Substances (PFAS). Environ Sci Process Impacts 22 (12), 2345–2373. https://doi.org/10.1039/D9EO002916.

Habimana, E., Sauvé, S., 2025. A review of properties, occurrence, fate, and transportation mechanisms of contaminants of emerging concern in sewage sludge, biosolids, and soils: recent advances and future trends. Front. Environ. Chem. 6, 1547596. https://doi.org/10.3389/fenvc.2025.1547596.

He, D., Zhu, T., Sun, J., Pan, X., Li, J., Luo, H., 2024. Emerging Organic Contaminants in Sewage Sludge: Current Status, Technological Challenges and Regulatory Perspectives. Sci. Total Environ. 955, 177234. https://doi.org/10.1016/j.scitotenv.2024.177234.

Hoïsæter, Å., Pfaff, A., Breedveld, G., 2019. Leaching and Transport of PFAS from Aqueous Film-Forming Foam (AFFF) in the Unsaturated Soil at a Firefighting Training Facility under Cold Climatic Conditions. J. Contam. Hydrol. 222, 112–122. https://doi.org/10.1016/j.conhyd.2019.02.010.

Kim Lazcano, R., Perre, C., Mashtare, M.L., Lee, L.S., 2019. Per- and Polyfluoroalkyl Substances in Commercially Available Biosolid-based Products: The Effect of Treatment Processes. Water Environ. Res. 91 (12), 1669–1677. https://doi.org/10.1002/wer.1174.

Klenow, S., Heinemeyer, G., Brambilla, G., Dellatte, E., Herzke, D., De Voogt, P., 2013. Dietary Exposure to Selected Perfluoroalkyl Acids (PFASs) in Four European Regions. Food Additives & Contaminants: Part A 30 (12), 2141–2151. https://doi.org/10.1080/19440049.2013.849006.

Krippner, J., Brunn, H., Falk, S., Georgii, S., Schubert, S., Stahl, T., 2014. Effects of Chain Length and pH on the Uptake and Distribution of Perfluoroalkyl Substances in Maize (Zea Mays). Chemosphere 94, 85–90. https://doi.org/10.1016/j.chemosphere.2013.09.018.

Lebrazzi, S., Frikari-Benrahim, K., 2022. Potential of Tree Legumes in Agroforestry Systems and Soil Conservation. In: Advances in Legumes for Sustainable Intensification. Elsevier, pp. 461–482. https://doi.org/10.1016/B978-0-323-85797-0.00004-5.

Lechner, M., Knapp, H., 2011. Carryover of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) from soil to plant and distribution to the different plant compartments studied in cultures of carrots (*Daucus carota* spp. *sativus*), potatoes (*Solanum tuberosum*), and cucumbers (*Cucumis sativus*). J. Agric. Food Chem. 59 (20), 11011–11018. https://doi.org/10.1021/jf201355y.

Lee, H., Tevlin, A.G., Mabury, S.A., Mabury, S.A., 2014. Fate of Polyfluoroalkyl Phosphate Diesters and Their Metabolites in Biosolids-Applied Soil: Biodegradation and Plant Uptake in Greenhouse and Field Experiments. Environ. Sci. Technol. 48 (1), 340–349. https://doi.org/10.1021/es403949z.

Lesmeister, L., Lange, F.T., Breuer, J., Biegel-Engler, A., Giese, E., Scheurer, M., 2021. Extending the Knowledge about PFAS Bioaccumulation Factors for Agricultural Plants - A Review. Sci. Total Environ. 766, 142640. https://doi.org/10.1016/j.scitotenv.2020.142640.

Link, G.W., Reeves, D.M., Cassidy, D.P., Coffin, E.S., 2024. Per- and Polyfluoroalkyl Substances (PFAS) in Final Treated Solids (Biosolids) from 190 Michigan Wastewater Treatment Plants. J. Hazard. Mater. 463, 132734. https://doi.org/10.1016/j.jhazmat.2023.132734.

Liu, Y., Hou, X., Chen, W., Kong, W., Wang, D., Liu, J., Jiang, G., 2019b. Occurrences of Perfluoroalkyl and Polyfluoroalkyl Substances in Tree Bark: Interspecies Variability Related to Chain Length. Sci. Total Environ. 689, 1388–1395. https://doi.org/10.1016/j.scitotenv.2019.06.454.

Liu, Z., Lu, Y., Shi, Y., Wang, P., Jones, K., Sweetman, A., Johnson, A., Zhang, M., Zhou, Y., Lu, X., Su, C., Sarvajayakesalvaluc, S., Khan, K., 2017a. Crop bioaccumulation and human exposure of perfluoroalkyl acids through multi-media transport from a mega fluorochemical industrial park, China. Environ. Int. 106, 37–47. https://doi.org/10.1016/j.envint.2017.05.014.

Liu, Z., Lu, Y., Shi, Y., Wang, P., Jones, K., Sweetman, A., Johnson, A., Zhang, M., Zhou, Y., Lu, X., Su, C., Sarvajayakesalvaluc, S., Khan, K., 2017b. Crop bioaccumulation and human exposure of perfluoroalkyl acids through multi-media transport from a mega fluorochemical industrial park, China. Environ. Int. 106, 37–47. https://doi.org/10.1016/j.envint.2017.05.014.

Liu, Z., Lu, Y., Song, X., Jones, K., Sweetman, A., Johnson, A., Zhang, M., Lu, X., Su, C., 2019a. Multiple crop bioaccumulation and human exposure of perfluoroalkyl substances around a mega fluorochemical industrial park, China: implication for planting optimization and food safety. Environ. Int. 127, 671–684. https://doi.org/10.1016/j.envint.2019.04.008.

Mayakaduwage, S., Ekanayake, A., Kurwadkar, S., Rajapaksha, A.U., Vithanage, M., 2022. Phytoremediation Prospects of Per- and Polyfluoroalkyl Substances: A Review. Environ. Res. 212, 113311. https://doi.org/10.1016/j.envres.2022.113311.

Mei, W., Sun, H., Song, M., Jiang, L., Li, Y., Lu, W., Ying, G.-G., Luo, C., Zhang, G., 2021. Per- and Polyfluoroalkyl Substances (PFASs) in the soil–plant system: sorption, root uptake, and translocation. Environ. Int. 156, 106642. https://doi.org/10.1016/j.envint.2021.106642.

Mejia-Avendaño, S., Munoz, G., Sauvé, S., Liu, J., 2017. Assessment of the Influence of Soil Characteristics and Hydrocarbon Fuel Contamination on the Solvent Extraction of Perfluoroalkyl and Polyfluoroalkyl Substances. Anal. Chem. 89 (4), 2539–2546. https://doi.org/10.1021/acs.analchem.6b04746.

Michaud, A., Mercier, V., Rampon, J.-N., Morvan, T., Burban, M., Montenach, D., Hammel, F., Sappin-Didier, V., Francoise, W., Feder, F., Paillat, J.-M., Masse, D., Hien, E., Bacheley, H., Houtot, S., 2013. SOERE PRO: Long Term Field Experiment Network for Research on the Recycling of Organic Matters Issued of Wastes in Agriculture.
Michaud, A.M., Cambier, P., Sappin-Didier, V., Deltreil, V., Mercier, V., Rampon, J.-N., Houot, S., 2020. Mass Balance and Long-Term Water Accumulation of Trace Elements in Arable Crop Systems Amended with Urban Composts or Cattle Mange during 17 Years. Environ. Sci. Pollut. Res. 27 (5), 5367–5386. https://doi.org/10.1007/s11356-019-07166-8.

Michaud, A.M., Sappin-Didier, V., Cambier, P., Nguyen, C., Janot, N., Montenach, D., Filipovic, L., Deltreil, V., Houot, S., 2021. Phytoavailability of Cd, Cr, Cu, Hg, Mn, Mo, Ni, Pb, Tl and Zn in arable crop systems amended for 13 to 15 years with organic waste products. Agronomy 11 (4), 664. https://doi.org/10.3390/agronomy11040664.

Michaud, A.M., Dunsin Saliu, T., Munoz, G., Feder, F., Sappin-Didier, V., Watteau, F., Houot, S., Sauvé, S., 2025. In Situ Occurrence and Mobility of per and Polyfluoroalkyl Substances in Soils Amended with Organic Waste Products. Sci. Total Environ. 984, 179708. https://doi.org/10.1016/j.scitotenv.2025.179708.

Moodie, D., Coggan, T., Berry, K., Kolobaric, A., Fernandes, M., Lee, E., Reichman, S., Nugegoda, D., Clarke, B.O., 2021. Legacy and Emerging Per- and Polyfluoroalkyl Substances (PFASs) in Australian Biosolids. Chemosphere 270, 129143. https://doi.org/10.1016/j.chemosphere.2020.129143.

Munoz, G., Ray, P., Mejia-Avendaño, S., Duy, S. vo, Do, D.T., Liu, J., Sauvé, S., 2018. Optimization of extraction methods for comprehensive profiling of perfluoroalkyl and polyfluoroalkyl substances in firefighting foam impacted soils. Anal. Chim. Acta 1034, 74–84. https://doi.org/10.1016/j.aca.2018.06.046.

Munoz, G., Michaud, A., Liu, M., Duy, S. vo, Montenach, D., Resseguier, C., Watteau, F., Sappin-Didier, V., Feder, F., Morvan, T., Houot, S., Desrosiers, M., Liu, J., Sauvé, S., 2021. Target and nontarget screening of PFAS in biosolids, composts, and other organic waste products for land application in France. Environ. Sci. Technol. https://doi.org/10.1021/acs.est.1c03697 null, null.

Navarro, I., De La Torre, A., Sanz, P., Porcel, M.A., Pro, J., Carbonell, G., Martínez, M.D. L.A., 2017a. Uptake of Perfluoroalkyl Substances and Halogenated Flame Retardants by Crop Plants Grown in Biosolids-Amended Soils. Environ. Res. 152, 199–206. https://doi.org/10.1016/j.envres.2016.10.018.

Navarro, I., de la Torre, A., Sanz, P., Porcel, M.A., Pro, J., Carbonell, G., Martínez, M. de los Á., 2017b. Uptake of perfluoroalkyl substances and halogenated flame retardants by crop plants grown in biosolids-amended soils. Environ. Res. 152, 199–206. https://doi.org/10.1016/j.envres.2016.10.018.

Nguyen, T.M.H., Bräunig, J., Thompson, C., Barnes, C.M., Higgins, C.P., McLaughlin, M.J., Mueller, J.F., 2020. Influences of chemical properties, soil properties, and solution pH on soil-water partitioning coefficients of per- and polyfluoroalkyl substances (PFASs). Environ. Sci. Technol. 54 (24), 15883–15892. https://doi.org/10.1021/acs.est.0c05705.

Pizzeghello, D., Bellin, L., Nardi, S., Francioso, O., Squartini, A., Concheri, G., 2021. Wood-Based Compost Affects Soil Fertility and the Content of Available Forms of Nutrients in Vineyard and Field-Scale Agroecosystems. Agronomy 11 (3), 518. https://doi.org/10.3390/agronomy11030518.

Poutanen, K.S., Kärlund, A.O., Gómez-Gallego, C., Johansson, D.P., Scheers, N.M., Marklinder, I.M., Eriksen, A.K., Silventoinen, P.C., Nordlund, E., Sozer, N., Hanhineva, K.J., Kolehmainen, M., Landberg, R., 2022. Grains – a Major Source of Sustainable Protein for Health. Nutr. Rev. 80 (6), 1648–1663. https://doi.org/10.1093/nutrit/nua084.

Qian, S., Lu, H., Xiong, T., Zhi, Y., Munoz, G., Zhang, C., Li, Z., Liu, C., Li, W., Wang, X., He, Q., 2023. Bioaccumulation of Per- and Polyfluoroalkyl Substances (PFAS) in Ferns: Effect of PFAS Molecular Structure and Plant Root Characteristics. Environ. Sci. Technol. 57 (11), 4443–4453. https://doi.org/10.1021/acs.est.2c06883.

RfD, U.S.E.P.A., 2022. Technical Fact Sheet: Drinking Water Health Advisories for Four PFAS (PFOA, PFOS, GenX Chemicals, and PFBS). https://www.epa.gov/system/files/documents/2022-06/technical-factsheet-four-PFAS.pdf.

Saliu, T.D., Sauvé, S., 2024. A review of per- and polyfluoroalkyl substances in biosolids: geographical distribution and regulations. Front. Environ. Chem. 5, 1383185. https://doi.org/10.3389/fenvc.2024.1383185.

Saliu, T.D., Liu, M., Habimana, E., Fontaine, J., Dinh, Q.T., Sauvé, S., 2024. PFAS Profiles in Biosolids, Composts, and Chemical Fertilizers Intended for Agricultural Land Application in Quebec (Canada). J. Hazard. Mater. 480, 136170. https://doi.org/10.1016/j.jhazmat.2024.136170.

Searce, A.E., Goossen, C.P., Schattman, R.E., Mallory, E.B., MacRae, J.D., 2023. Linking drivers of plant per- and polyfluoroalkyl substance (PFAS) uptake to agricultural land management decisions. Biointerphases 18 (4), 040801. https://doi.org/10.1116/6.0002772.

Sepulvado, J.G., Blaine, A.C., Hundal, L.S., Higgins, C.P., 2011. Occurrence and Fate of Perfluorochemicals in Soil Following the Land Application of Municipal Biosolids. Environ. Sci. Technol. 45 (19), 8106–8112. https://doi.org/10.1021/es103903d.

Shahbandeh, M., 2025. Statista: Global Wheat Consumption 2017/18-2024/25. https://www.statista.com/statistics/1094056/total-global-rice-consumption/.

Sivaram, A.K., Panneerselvan, L., Surapaneni, A., Lee, E., Kannan, K., Megharaj, M., 2022. Per- and Polyfluoroalkyl Substances (PFAS) in Commercial Composts, Garden

Soils, and Potting Mixes of Australia. Environmental Advances 7, 100174. https://doi.org/10.1016/j.envadv.2022.100174.

Sivaram, A.K., Lee, E., Curnow, A., Surapaneni, A., Kannan, K., Megharaj, M., 2023. Uptake, Accumulation, and Toxicity of per- and Polyfluoroalkyl Substances in Allium Cium Grown in Soils Amended with Biosolids. Environmental Challenges 10, 100670. https://doi.org/10.1016/j.envc.2022.100670.

SOERE PRO, 2015. https://valor-pro.hub.inrae.fr/ accessed 2025-04-19.

Statista Research Department, 2024. https://fr.statista.com/statistiques/537414/ble-ten-dre-variation-consommation-humaine-france/ accessed 2024-07-04.

Tavakkoli, E., Rengasamy, P., Smith, E., McDonald, G.K., 2015. The effect of cation-anion interactions on soil pH and solubility of organic carbon. Eur. J. Soil Sci. 66 (6), 1054–1062. https://doi.org/10.1111/ejs.12294.

Torres, F.G., De-la-Torre, G.E., 2023. Per- and Polyfluoroalkyl Substances (PFASs) in Consumable Species and Food Products. J. Food Sci. Technol. 60 (9), 2319–2336. https://doi.org/10.1007/s13197-022-05545-7.

UNEP, 2009. Report of the Conference of the Parties of the Stockholm Convention on Persistent Organic Pollutants on the Work of Its Fourth Meeting. UNEP/POPS/COP.4/38. https://www.pops.int/ (accessed 2025-07-04).

USEPA, 2024. Biden-Harris Administration Finalizes First-Ever National Drinking Water Standard to Protect 100M People from PFAS Pollution. https://www.epa.gov/ newsreleases/biden-harris-administration-finalizes-first-ever-national-drinking-water-standard#:~:text=PA20is%20setting%20enforceable%20Maximum,are%20fe asible%20for%20effective%20implementation accessed 2024-05-17.

USEPA PFAS RfD, 2016. Technical Fact Sheet – Perfluorooctane Sulfonate (PFOS) and Perfluorooctanoic Acid (PFOA). https://19january2021snapshot.epa.gov/sites/stat ic/files/2017-12/documents/ffrrofactsheet_contaminants_pfoa_pfoa_11-20-17_508 _0.pdf accessed 2025-05-08.

Wang, W., Rhodes, G., Ge, J., Yu, X., Li, H., 2020. Uptake and Accumulation of Per- and Polyfluoroalkyl Substances in Plants. Chemosphere 261, 127584. https://doi.org/10.1016/j.chemosphere.2020.127584.

Wang, W., Yuan, S., Kwon, J.-H., 2022. Insight into the Uptake and Translocation of Per- and Polyfluoroalkyl Substances in Hydroponically Grown Lettuce. Environ. Sci. Pollut. Res. 29, 85454–85464. https://doi.org/10.1007/s11356-022-21886-4.

Wen, B., Li, L., Zhang, H., Ma, Y., Shan, X.-Q., Zhang, S., 2014a. Field Study on the Uptake and Translocation of Perfluoroalkyl Acids (PFASs) by Wheat (Triticum aestivum L.) Grown in Biosolids-Amended Soils. Environ. Pollut. 184, 547–554. https://doi.org/10.1016/j.envpol.2013.09.040.

Wen, B., Li, L., Zhang, H., Ma, Y., Shan, X.-Q., Zhang, S., 2014b. Field Study on the Uptake and Translocation of Perfluoroalkyl Acids (PFASs) by Wheat (Triticum aestivum L.) Grown in Biosolids-Amended Soils. Environ. Pollut. 184, 547–554. https://doi.org/10.1016/j.envpol.2013.09.040.

Wen, B., Wu, Y., Zhang, H., Liu, Y., Hu, X., Huang, H., Zhang, S., 2016. The Roles of Protein and Lipid in the Accumulation and Distribution of Perfluorooctane Sulfonate (PFOS) and Perfluorooctanoate (PFOA) in Plants Grown in Biosolids-Amended Soils. Environ. Pollut. 216, 682–688. https://doi.org/10.1016/j.envpol.2016.06.032.

Wen, B., Pan, Y., Shi, X., Zhang, H., Hu, X., Huang, H., Lv, J., Zhang, S., 2018. Behavior of N-Ethyl Perfluorooctane Sulfonamido Acetic Acid (N-EtFOSAA) in Biosolids Amended Soil-Plant Microcosms of Seven Plant Species: Accumulation and Degradation. Sci. Total Environ. 642, 366–373. https://doi.org/10.1016/j. scitotenv.2018.06.073.

Xu, B., Qiu, W., Du, J., Wan, Z.-X., Zhou, J.L., Chen, H., Liu, R., Magnuson, J.T., Zheng, C., 2022. Translocation, Bioaccumulation, and Distribution of Perfluoroalkyl and Polyfluoroalkyl Substances (PFASs) in Plants. iScience 25. https://doi.org/10.1016/j.isci.2022.104061 null.

Xu, K., Huang, J., Zhang, Y., Wu, X., Cai, D., Hu, G., Li, Y., Ni, Z., Lin, Q., Wang, S., Qiu, R., 2024. Crop Contamination and Human Exposure to Per- and Polyfluoroalkyl Substances around a Fluorocheological Industrial Park in China. Toxics 12 (4), 269. https://doi.org/10.3390/toxics12040269.

Yang, H., Zhao, Y., Chai, L., Ma, F., Yu, J., Xiao, K.-Q., Gu, Q., 2024. Bio-Accumulation and Health Risk Assessments of per- and Polyfluoroalkyl Substances in Wheat Grains. Environ. Pollut. 356, 124351. https://doi.org/10.1016/j.envpol.2024.124351.

Zhang, H., Vestergren, R., Wang, T., Yu, J., Jiang, G., Herzke, D., 2017. Geographical Differences in Dietary Exposure to Perfluoroalkyl Acids between Manufacturing and Application Regions in China. Environ. Sci. Technol. 51 (10), 5747–5755. https://doi.org/10.1021/acs.est.7b00246.

Zhang, W., Cao, H., Liang, Y., 2021a. Plant Uptake and Soil Fractionation of Five Ether- PFAS in Plant-Soil Systems. Sci. Total Environ. 771, 144805. https://doi.org/10.1016/j.scitotenv.2020.144805.

Zhang, W., Cao, H., Liang, Y., 2021b. Plant Uptake and Soil Fractionation of Five Ether- PFAS in Plant-Soil Systems. Sci. Total Environ. 771, 144805. https://doi.org/10.1016/j.scitotenv.2020.144805.

Zhu, H., Kannan, K., 2019. Distribution and Partitioning of Perfluoroalkyl Carboxylic Acids in Surface Soil, Plants, and Earthworms at a Contaminated Site. Sci. Total Environ. 647, 954–961. https://doi.org/10.1016/j.scitotenv.2018.08.051.