N Sertillanges

C.-S Haudin

M Bourdat-Deschamps

N Bernet

V Serre

A Danel

S Houot

D Patureau

Process type is the key driver of the fate of organic micropollutants during industrial scale treatment of organic wastes

Keywords: Anaerobic digestion, composting, dewatering, liming, organic micropollutants, reduction rates ACTC, anhydrochlortetracycline, ANT, anthracene, ATC, anhydrotetracycline, BAA, benzo(a)anthracene, BAP, benzo FLO, fluoranthene, FLQ, flumequine, FLU, fluorene, FLX, fluoxetine, GEM, gemfibrozil, IBU, ibuprofen, IM, inorganic matter, IND, indeno nonylphenol monoethoxylate, NP2EO, nonylphenol diethoxylate, NPs, nonylphenols, OFL, ofloxacin, OMP, organic micropollutant, OTC, oxytetracycline, OW, organic waste, PAHs, polycyclic aromatic hydrocarbons, PHE, phenanthrene, PP, pharmaceutical product, PYR, pyrene, SPI, spiramycin, TC, tetracycline, TMP, trimethoprim, TRC, triclocarban, TRI, triclosan

Highlights

• New organic micropollutant-organic waste combinations assessed on treatment lines

• Fate driven by process type and compound specific behaviour

• Biological processes were more efficient than physicochemical ones

• Process combination enhanced most organic micropollutants dissipation

Introduction

Organic micropollutants (OMPs) such as pharmaceutical products (PPs), polycyclic aromatic hydrocarbons (PAHs) and nonylphenols (NPs, coming from the transformation of detergents named nonylphenol ethoxylates), have been quantified at ppb to ppm concentration levels in the ever growing quantity of organic wastes (OWs) around the world, e.g. in sewage sludge [START_REF] Clarke | Review of "emerging" organic contaminants in biosolids and assessment of international research priorities for the agricultural use of biosolids[END_REF][START_REF] Bergé | Metaanalysis of environmental contamination by alkylphenols[END_REF][START_REF] Verlicchi | Pharmaceuticals and personal care products in untreated and treated sewage sludge: Occurrence and environmental risk in the case of application on soil -A critical review[END_REF], in manure [START_REF] Youngquist | Fate of antibiotics and antibiotic resistance during digestion and composting: A review[END_REF][START_REF] Wohde | Occurrence and transformation of veterinary pharmaceuticals and biocides in manure: a literature review[END_REF][START_REF] Spielmeyer | Occurrence and fate of antibiotics in manure during manure treatments: A short review[END_REF][START_REF] Ghirardini | A review of the occurrence of selected micropollutants and microorganisms in different raw and treated manure -Environmental risk due to antibiotics after application to soil[END_REF] or territorial mixes (Brändli et al., 2007;[START_REF] Suominen | Hazardous organic compounds in biogas plant end products-Soil burden and risk to food safety[END_REF]. OMPs may come from direct human or animal excretion of PPs in waste after medication, atmospheric deposits, rain wash-off of hydrocarbons, domestic and industrial effluents loaded with surfactants, detergents etc. Agricultural land application for fertilization is one of the main ways to dispose of those wastes [START_REF] Mininni | EU policy on sewage sludge utilization and perspectives on new approaches of sludge management[END_REF], directly introducing potentially threatening OMPs into soil, that could be transferred in some cases to surface and/or ground waters. Before application, OWs may undergo biological treatments such as anaerobic digestion and composting or physico-chemical ones like dewatering or liming, to stabilise, sanitise the matter and concentrate useful nutrients. Combinations of these treatment processes are possible. Understanding the fate of OMPs during the OW treatments is important to evaluate and reduce the threat associated with OW land spreading.

All OW treatment processes have an effect on some of the OMPs present in wastes: anaerobic digestion and composting as biological treatment processes are known to dissipate or degrade PPs [START_REF] Ezzariai | Human and veterinary antibiotics during composting of sludge or 26 manure: Global perspectives on persistence, degradation, and resistance genes[END_REF][START_REF] Wohde | Occurrence and transformation of veterinary pharmaceuticals and biocides in manure: a literature review[END_REF][START_REF] Spielmeyer | Occurrence and fate of antibiotics in manure during manure treatments: A short review[END_REF], nonylphenol ethoxylates and NP [START_REF] Zheng | Impact of composting strategies on the degradation of nonylphenol in sewage sludge[END_REF][START_REF] Spielmeyer | Occurrence and fate of antibiotics in manure during manure treatments: A short review[END_REF] and PAHs (Brändli et al., 2007;[START_REF] Aemig | Distribution of Polycyclic Aromatic Hydrocarbons (PAHs) in sludge organic matter pools as a driving force of their fate during anaerobic digestion[END_REF]. The effect of these treatment processes has been shown in lab and pilot scale experiments [START_REF] Phan | The fate of trace organic contaminants during anaerobic digestion of primary sludge: A pilot scale study[END_REF] for sludge anaerobic digestion; [START_REF] Spielmeyer | Elimination patterns of worldwide used sulfonamides and tetracyclines during anaerobic fermentation[END_REF] for manure anaerobic digestion; [START_REF] Geng | Impact of liming and drying municipal sewage sludge on the amount and availability of 14C-acetyl sulfamethoxazole and 14C-acetaminophen residues[END_REF] for sludge drying and liming) and in some studies where in situ sampling was performed on industrial sites [START_REF] Lillenberg | Presence of fluoroquinolones and sulfonamides in urban sewage sludge and their degradation as a result of composting[END_REF] for sludge composting; Martin et al. (2015) for sludge anaerobic digestion and composting; [START_REF] Mailler | Fate of emerging and priority micropollutants during the sewage sludge treatment: Case study of Paris conurbation. Part 1: Contamination of the different types of sewage sludge[END_REF] for sludge anaerobic digestion), each time for a small selection of micropollutants. The impact of OW origin and type on the fate of OMPs during the treatment processes has been poorly documented especially for some OMP families and for wastes coming from territorial sources, mostly comprising mixes of wastes. To the best of our knowledge, a wide in situ study on OMP fate during OW treatment with unified quantification methods to identify global trends has not been tried before.

This study focuses on the impact of OW treatment on the fate of 53 OMPs along 10 industrial treatment lines treating urban, agricultural wastes or mixture of both OW types. The combination of studying a diversity of OWs, a diversity of OMPs with different characteristics (solubility, ionic charges, hydrophobicity etc.), sampling in situ industrial sites, quantifying native OMP concentrations and looking at complete treatment lines allows for a global and representative view of the OMP fate in the French OW treatment sector.

Material and Methods

Organic micropollutants, sites and organic waste treatment processes

Thirty-five pharmaceutical products, 2 biocides, 3 nonylphenols and 13 polycyclic aromatic hydrocarbons (Table S1; Supplementary Information, SI) with diverse chemical properties in terms of sorption and transformation (Table S2, SI) were selected to highlight contrasted fate during treatment processes. Due to the study of various organic wastes, OMPs were also selected based on their frequent (co)occurrence in sludge, manure, food waste, green waste if data is available.

Ten sites located in different parts of France and in La Reunion Island were selected for their processes and their input feeding waste diversity from agricultural, territorial or urban origins. Sites were representative of most common types of organic wastes and treatment processes in France, i.e. anaerobic digestion, composting, drying and liming (Table 1 andFigure S1). Agricultural sites (Agri I-IV, Table 1) included two farm-size solid batch anaerobic digestion units treating bovine manure, one continuous liquid anaerobic digestion unit only treating pig manure and one experimental research site directly composting cow manure. Territorial sites (Terri I-III) were industrial continuous liquid anaerobic digestion units treating mixtures of agro-industrial waste, liquid pig manure, sewage sludge, cereal, food waste etc. Urban sites (Urb I-III) were wastewater treatment plants processing sludge by either anaerobic digestion in mesophilic or thermophilic conditions, composting or both treatments. A single substrate (the waste undergoing the treatment) could undergo a series of treatment processes (Process continuity, Table 1 andFigure S1). Samples were taken the same day along the waste treatment line, before and after each treatment step including drying and phase separation. For heterogeneous solid matrices (e.g. manure, compost), up to ten sub-samples from different places were gathered to obtain a composite and representative sample of 5 to 8 kg (dry mass). For more homogenous liquid samples, 3 to 15 L, depending on total solid content, were sampled in stirred tanks to get a representative sample. All samples were stored at -20°C on sampling day or the day after.

Analytical methods

Dry matter (DM) and volatile solid (VS) contents were measured in duplicates by mass difference after 24h at 105°C and after additional 2h at 550°C respectively. The remaining ashes were considered as inorganic matter (IM).

PAHs and NPs

Raw samples were frozen at -80°C then freeze-dried for a week and grinded (Table S1, SI).

PAHs and NPs were extracted from one gram subsample according to [START_REF] Trably | Statistical tools for the optimization of a highly reproducible method for the analysis of polycyclic aromatic hydrocarbons in sludge samples[END_REF] and [START_REF] Mailler | Fate of emerging and priority micropollutants during the sewage sludge treatment: Case study of Paris conurbation. Part 1: Contamination of the different types of sewage sludge[END_REF]. Control matrices with known concentration of NPs/PAHs were extracted in parallel.

Solvent extracts were then evaporated and dissolved in either 100% acetonitrile for PAHs or 100% hexane for NPs. Each extract was analysed with a Waters Alliance 2695 High-Performance-Liquid-Chromatography with a fluorescence detector. Conditions of separation and detection are specified in Table S1 (SI). Each sample was extracted twice and each extract quantified twice, giving a total of 4 values. Limits of quantification (LOQs) were estimated from the lowest points in calibration curves: 5 µg/L for PAHs, 100 µg/L for NPs in extracts.

Pharmaceutical products

All samples were analysed in triplicates. Briefly, solid samples were spiked with a mixture of internal deuterated-labelled standards, left overnight and extracted as described in Table S1 according to [START_REF] Ferhi | Factors influencing the extraction of pharmaceuticals from sewage sludge and soil: an experimental design approach[END_REF]. The supernatants were purified after centrifugation with a modified QuEChERS method [START_REF] Ferhi | Factors influencing the extraction of pharmaceuticals from sewage sludge and soil: an experimental design approach[END_REF]. Liquid samples (DM <20%) were centrifuged at 18600 g for 20 min. The obtained solid phase was extracted as mentioned above. The liquid phase was spiked with a mixture of internal deuterated-labelled standards and purified using the modified QuEChERS method [START_REF] Bourdat-Deschamps | Multi-residue analysis of pharmaceuticals in aqueous environmental samples by online solid-phase extraction-ultra-high-performance liquid chromatography-tandem mass spectrometry: Optimisation and matrix effects reduction by quick, easy, cheap, effective, rugged and safe extraction[END_REF]. Pharmaceuticals were analysed with online Solid-Phase-Extraction and Ultra-High-Performance-Liquid-Chromatography coupled with a triple quadrupole mass spectrometer (Table S1). The compound concentrations were determined by internal quantificationisotope dilution in order to correct both extraction/purification losses and potential matrix effects in mass spectrometry (MS). For this study, 23 compounds were added to the published analytical method, with MS-MS transitions detailed in Table S3 (SI); trueness recoveries and intra-day precision are detailed in Table S4 (SI). LOQs for each compound and each extracted matrix were estimated as the concentration corresponding to a signal-to-noise ratio of ten. Limits of detection (LODs) were considered equal to LOQ/3. Concentrations between LOD and LOQ values were taken equal to LOQ/2 for statistical analysis. For liquid samples, only the concentrations in the solid fraction were considered since PP concentrations in liquid phases were often very low or below LOQ or LOD values.

Data treatment and analysis

Mean concentrations

Micropollutant concentrations were first expressed in µg/kg DM. Results were considered to follow a normal distribution and the probability of having more than one outlier to be very low with only 3 or 4 values. Outliers were identified with a two tailed Dixon's Q test [START_REF] Dean | Simplified Statistics for Small Numbers of Observations[END_REF] with a 95% confidence threshold using [START_REF] Rorabacher | Statistical Treatment for Rejection of Deviant Values : Critical Values of Dixon ' s " O " Parameter and Related Subrange Ratios at the 95 % Confidence Level[END_REF]'s modifications (for 3 and 4 values, Q= 0.97 and 0.829 respectively) and discarded before mean and standard deviation calculations.

Correction of output pollutant concentrations

Changes in OMP concentration along a given process were characterised using IM as comparing point [START_REF] Zheng | Biodegradation of nonylphenol during aerobic composting of sewage sludge under two intermittent aeration treatments in a full-scale plant[END_REF], since IM was considered stable along the studied processes whereas organic matter could evolve during some processes. Output OMP concentrations were adjusted as follows.

out, corr = out, m out in where [OMP]out, corr, is the corrected OMP concentration, [OMP]out, m the measured concentration, IMin and IMout the % of IM in input and output respectively. This correction was not applicable for dewatering processes due to the possible loss of IM in the liquid fractions (not quantified). However, dissipation rates (section 2.4.3.) were calculated for these dewatering processes assuming a loss of low amounts of IM. The results on dewatering processes were only compared between themselves to highlight the partition behaviour of OMPs.

Pollutant dissipation rates and heat map

For each OMP and process, the input and corrected output concentrations were compared using a two-sample unequal variance (heteroscedastic) Student's T test, with a two tail distribution computed with Excel. When different (p-value < 0.05), dissipation rates could be calculated.

(%) = - , 100
Four classes of dissipation rates were considered in a heat map gathering all results: no significant change, up to 30%, 30-70% and over 70%. The "+" sign indicated a higher OMP concentration in the output, "nc" a non-calculable rate with non-detectable contents or detectable with no available LOQ value in the output and the input, "*" the absence of data.

For Urb II composting, OMP dissipation rate was calculated considering raw sludge (input)

and final compost (output). Since the composting initial mixture (raw sludge, green waste) was not sampled, its characteristics were assessed using DM/VS ratio from a generic green waste and a raw sludge/green waste mass ratio of 33/66. For Urb III liming, the dissipation rate was established between dried digested sludge (input) and limed pellets (output), considering a 20% mass dilution through CaO addition.

Spiramycin (SPI) was not displayed in Figure 2, its values being only semi-quantitative.

The chosen sampling method, i.e. sampling the process input and output on the same day, without considering the process time (from hours and days for centrifugation, drying, liming to several days and weeks for anaerobic digestion and composting), implies that the resulting dissipation rates can be impacted by a temporal variability of the input or output OMP content. This is particularly true for the biological processes with long running time. There are very few data on the time variability of the OMP contents in OW treatments by comparison to the one provided for water treatment and its impact on OMP removal assessment [START_REF] Verlicchi | Occurrence of micropollutants in wastewater and evaluation of their removal efficiency in treatment trains: The influence of the adopted sampling mode[END_REF]. Mailler et al.

(2017) provided variation coefficients of 50-150% for some OMP (mainly PP) concentrations in raw sludge sampled 2 times over 4 consecutive weeks at 2 wastewater treatment plants (WWTP). When considering only one WWTP, these coefficients were fully reduced; they were also lower for digested sludge and very low for persistent compounds (PAHs, NPs) whatever the type of sludge. This could be linked to the sludge age entering sludge processes (around 8-10 days depending on water treatment)

and to the presence of storage tanks that are usually present to regulate loads of processes; sludge age and storage could play the role of buffer media. In the present study, the calculated dissipation rates will only be considered as apparent and not as formal ones. Furthermore, these rates are displayed as wide classes, lowering the impact of time variability and only general trends will be discussed according to process and OW types.

Results and discussion

As expected, all biological and dewatering processes were representative of efficient waste treatments, given the removal efficiencies of volatile matter (Table 1) and water (Table S5, SI). Urb III liming led to a 3 fold increase in Ca content following CaO addition.

Ten PPs out of 37 were never detected in all samples: 6 antibiotics (sulfamethazine, sulfamethoxazole, sulfamerazine, sulfachloropyridazine, n-acetyl sulfamethoxazole; tylosin B) and 4

other PPs (ivermectin, eprinomectin, ketoprofene, acetamidophenol). Moreover, five PPs were detected or quantified in a few OWs (marbofloxacin, sulfadiazine, lincomycin, levamisole and flunixine). The results for these PPs are not presented in this article.

In the following parts, the term "setting" is used to characterise the waste origin (Agricultural, Territorial or Urban) while "site" is used for a single location where several processes can take place. "Process" refers to only one organic waste treatment at a time, i.e. anaerobic digestion or composting.

Micropollutants in process input substrate

OMP input concentrations are displayed in Table S6 (SI) giving only values above LOQ. (OMP output concentrations are displayed in Table S7 (SI), as a comparing point).

Fluoroquinolones, macrolides and other PPs (including biocides) were more specific to Urb sites (Figure 1) than tetracyclines. PAHs and NPs were ubiquitous with detection occurrences above 70% whatever the site type.

Antibiotics

Quinolones

Fluoroquinolones were weakly quantified in Agricultural (3/25) and Territorial (4/15) settings (Table S6, SI), in accordance with limited veterinary uses in France since March 2016. Only two compounds were quantified on Agri I site: a) Enrofloxacin (ENR) in anaerobic digestion substrate and resulting composting initial mixture and b) Ciprofloxacin (CIP) in anaerobic digestion substrate. ENR is only authorised for poultry, pets and pigs and CIP for humans. CIP is also a metabolite of ENR degradation [START_REF] Martinez | Pharmacology of the fluoroquinolones: A perspective for the use in domestic animals[END_REF], explaining its lower concentration than those in other settings.

Norfloxacin (NOR), Ofloxacin (OFL) and CIP, prescribed in human medicine and only to pet and equine animals in restricted conditions, were mainly quantified in samples with sewage sludge: nearly all the Urb anaerobic digestion and composting samples (up to several mg/kg DM) and the Terri II anaerobic digestion substrate (28% of sewage sludge, Table 1) with concentrations always inferior, strengthening the idea of the sludge contribution to the total amount of these compounds in initial mixtures. Flumequine (FLQ) was only quantified in small quantities in two Urb composting substrates which is well correlated with its lower use in human medicine. As already reported [START_REF] Clarke | Review of "emerging" organic contaminants in biosolids and assessment of international research priorities for the agricultural use of biosolids[END_REF]Peysson and Vuillet, 2013;Mailler et al., 2016;[START_REF] Bourdat-Deschamps | Fate and impacts of pharmaceuticals and personal care products after repeated applications of organic waste products in long-term field experiments[END_REF], the highest levels of fluoroquinolones and quinolones were quantified in human-related substrates.

Tetracyclines

Among all PPs, tetracyclines were the most abundant and frequently detected compounds in all settings (Figure 1, table S6, SI). Tetracyclines are widely used in both human and veterinary medicines. Samples from Agri settings, in particular Agri I site, contained the highest diversity of tetracyclines and highest contents for some compounds. Samples from territorial setting had concentrations usually in-between urban and agricultural values, making sense according to the substrate composition (Table 1). The concentrations of chlortetracycline (CTC-ECTC) in the anaerobic digestion and composting Agri I substrates reached nearly 15000 µg/kg DM, in line with [START_REF] Spielmeyer | Occurrence and fate of antibiotics in manure during manure treatments: A short review[END_REF][START_REF] Spielmeyer | Simultaneous determination of 14 sulfonamides and tetracyclines in biogas plants by liquid-liquid-extraction and liquid chromatography tandem mass spectrometry[END_REF] and [START_REF] Zhou | Excretion masses and environmental occurrence of antibiotics in typical swine and dairy cattle farms in China[END_REF]. CTC-ECTC was found on sites where pig manure was treated (Agri I and Terri I) but not on sites treating waste of human or bovine origin, in accordance with its wide use in porcine populations for digestive and respiratory infections and its prescription in very specific conditions otherwise, e.g. cutaneous infections (humans) and calving disorders (cows).

Oxytetracycline (OTC), withdrawn from the health market in France in 2002, was also only quantified in Agri I and Terri I samples, containing pig manure. Low concentration levels could be explained by a rapid transformation of OTC reported in other contexts, e.g. a 6.5 day half-life (hydrolysis) at 25°C in aqueous environment with an optimum at neutral pH [START_REF] Xuan | Hydrolysis and photolysis of oxytetracycline in aqueous solution[END_REF]. Dehydrated degradation products of tetracycline (TC) and CTC-ECTC, anhydrotetracycline (ATC) and anhydrochlortetracycline (ACTC), respectively, were often quantified when their parent compounds were also present in the samples. ATC concentrations were close or superior to TC ones in all settings; this was often the same for ACTC and CTC. Doxycycline (DOX), used in both veterinary and human medicines, was found in all urban samples with the highest amount at 9281 µg/kg DM, in 2 out of the 3 territorial anaerobic digestion substrates, with pig manure (2440-4923 µg/kg DM) and only in the Agri I composting sample, with pig manure (2277 µg/kg DM). This molecule was already found in high quantities in pig manure [START_REF] Bourdat-Deschamps | Fate and impacts of pharmaceuticals and personal care products after repeated applications of organic waste products in long-term field experiments[END_REF][START_REF] Ho | Occurrence of veterinary antibiotics and progesterone in broiler manure and agricultural soil in Malaysia[END_REF] but was barely reported in sludge samples.

Sulfonamides and Trimethoprim

Sulfonamides were not detected, in accordance with their low prescription, i. Its presence in organic waste could be an indicator of a small residual use of sulfamethoxazole.

Macrolides

Comparatively to other antibiotics, macrolides were only detected in small amounts, mirroring their low use for medicine and veterinary use in France (WHO Report on Surveillance of Antibiotic Consumption, 2018 and ANSES Report on veterinary antibiotics sales, 2019). Tylosin (TYL) not authorised for human use was only quantified in samples with pig manure. The low levels of TYL in samples could be explained by its fast biotic or abiotic degradation observed in other contexts [START_REF] Ingerslev | Biodegradability of metronidazole, olaquindox, and tylosin and formation of tylosin degradation products in aerobic soil-manure slurries[END_REF][START_REF] Liu | Dissipation of sulfamethoxazole, trimethoprim and tylosin in a soil under aerobic and anoxic conditions[END_REF][START_REF] Kolz | Degradation and Metabolite Production of Tylosin in Anaerobic and Aerobic Swine-Manure Lagoons[END_REF]. Erythromycin (ERY) was only quantified in urban sites in small quantities: 16-63 µg/kg DM. Spiramycin (SPI) was quite abundant in Terri settings even though results were semi-quantitative. Both compounds are used for human medicine and veterinary use.

Other pharmaceuticals and biocides

Of all other PPs, triclosan (TRI), a rather persistent human and veterinary biocide, was the most abundant compound found in all settings, in particular Agri I site (≈2300 µg/kg DM), Urb II site (≈5900 µg/kg DM), and Terri II site (≈1720 µg/kg DM) treating waste from activities where TRI could be used for hygiene purposes. A small quantity of triclocarban (TRC), another persistent antifungal biocide [START_REF] Lozano | Fate of triclocarban in agricultural soils after biosolid applications[END_REF], was detected in the three urban sites. Ogunyoku and Young (2008) found similar and higher amounts in urban sludge for TRI and TRC; no literature data was available for agricultural and territorial settings. Fluoxetine (FLX) and carbamazepine (CBZ) were only found in samples containing sludge, e.g. all Urb sites and Terri II site (23-338 µg/kg DM). FLX and CBZ are mostly prescribed to humans as antidepressant and anti-epileptic drugs. Diclofenac (DIC) was only quantified in urban samples as a compound authorised only for medicine use in France. In comparison ibuprofen (IBU) was found in samples from all settings, yet in small quantities (15-341 µg/kg DM), due to its wide use as active ingredient in human medicine and veterinary one for pets in France. Gemfibrozil (GEM), a hypolipidemic agent only prescribed to humans was found in all raw urban sludge below 28 µg/kg DM.

NPs

Concentrations of nonylphenol (NP) and nonylphenol polyethoxylates (NPEOs; Nonylphenol monoethoxylate, NP1EO; Nonylphenol diethoxylate, NP2EO) were higher than PP ones in all settings, often above 1000 µg/kg DM and up to 176000 µg/kg DM for NP1EO in Terri I anaerobic digestion input substrate. NP1EO was the most abundant compound in all territorial and urban sites and less present and concentrated in most agricultural samples except Agri IV input substrate. NPs were often detected in urban sludge, at similar concentrations [START_REF] Mailler | Priority and emerging pollutants in sewage sludge and fate during sludge treatment[END_REF][START_REF] Lawal | Polycyclic aromatic hydrocarbons. A review[END_REF]. NP2EO was less present than NP1EO, except in the Agri I input substrate. NP2EO and NP were absent from Territorial samples. NPEOs as industrial surfactants and detergents [START_REF] Bergé | Metaanalysis of environmental contamination by alkylphenols[END_REF]) may be recovered in urban and territorial settings. Their presence in agricultural samples was rarely documented especially at these concentration levels. [START_REF] Mortensen | Degradation of nonylphenol in spiked soils and in soils treated with organic waste products[END_REF] and [START_REF] Petersen | Recycling of sewage sludge and household compost to arable land: Fate and effects of organic contaminants, and impact on soil fertility[END_REF] reported a total NPs content respectively below 0.1 mg/kg DM and 0.5 mg/kg DM in pig manure. Since NP mainly comes from NPEOs degradation [START_REF] Ahel | Behaviour of alkylphenol polyethoxylate surfactants in the aquatic environment-II. Occurrence and transformation in rivers[END_REF]) and is more persistent, the relative low amount of NP or its non-detection in these process input samples seems to indicate a lack of time and/or inadequate conditions for the degradation of NPEOs.

PAHs

Although in smaller quantities than NPs and PPs, most of the 13 PAHs were detected in all samples with contents up to 340 µg/kg DM. Inputs of urban sites were the most contaminated in quantity and diversity followed by those of territorial sites and agricultural sites. PAHs are residues of incomplete combustion of organic fuel (wood, gasoline…) mostly produced by transportation, housing or industrial activities [START_REF] Lawal | Polycyclic aromatic hydrocarbons. A review[END_REF], explaining the higher quantities in urban and territorial samples than in agricultural ones. Concentrations were consistent with values reported by [START_REF] Mailler | Priority and emerging pollutants in sewage sludge and fate during sludge treatment[END_REF][START_REF] Mailler | Fate of emerging and priority micropollutants during the sewage sludge treatment: Case study of Paris conurbation. Part 1: Contamination of the different types of sewage sludge[END_REF] and [START_REF] Stevens | PAHs, PCBs, PCNs, organochlorine pesticides, synthetic musks, and polychlorinated n-alkanes in U.K. sewage sludge: Survey results and implications[END_REF]. In all sites, two or three aromatic cycle PAHs, mainly Phenanthrene (PHE), Fluoranthene (FLO), Pyrene (PYR), Chrysene (CHR), were the most abundant compounds. Concentrations of four or five cycle PAHs were usually 2 to 10 times lower than those of smaller PAHs. This PAH pattern is commonly found in sewage sludge [START_REF] Blanchard | Polycyclic aromatic hydrocarbons and polychlorobiphenyls in wastewaters and sewage sludges from the Paris area (France)[END_REF]. Even if

PAHs are very hydrophobic compounds, they were quantified at lower concentrations than those of some polar PPs (fluoroquinolones) that concentrated in the OWs due to charge interactions.

Impact of treatment process and substrate type on pollutant fate

Anaerobic digestion

Figure 2 contains OMP dissipation rates for each individual process considering the following scale: Low: 0-30%, Moderate: 30-70%, High: >70%. Anaerobic digestion had a positive effect on fluoroquinolones and quinolone with the highest dissipation rates (>70%) for urban processes with high input concentrations, and for Agri I anaerobic digestion. There was more variability in Terri processes except for CIP that accumulated on all sites which could come from ENR possible degradation [START_REF] Martinez | Pharmacology of the fluoroquinolones: A perspective for the use in domestic animals[END_REF]. CIP is a known ENR degradation product. ENR underwent either no change or was detected but not quantified, preventing any removal calculation except for Agri I.

Tetracyclines were only dissipated in territorial and agricultural settings. In all settings, when quantified, there was no real trend for TC and CTC-ECTC whereas ATC and ACTC presented high rates in some Agri and Terri sites. Mesophilic or thermophilic anaerobic digestion was shown to dissipate TC and CTC-ECTC in swine manure with reduction rates at 75-99% for CTC [START_REF] Varel | Effect of anaerobic digestion temperature on odour, coliforms and chlortetracycline in swine manure or monensin in cattle manure[END_REF][START_REF] Arikan | Degradation and metabolization of chlortetracycline during the anaerobic digestion of manure from medicated calves[END_REF][START_REF] Withey | Depletion of hormones and antimicrobials in cattle manure using thermophilic anaerobic digestion[END_REF] and 50-99% for TC [START_REF] Shi | Effect of antibiotics on methane arising from anaerobic digestion of pig manure[END_REF][START_REF] Cetecioglu | Chronic impact of tetracycline on the biodegradation of an organic substrate mixture under anaerobic conditions[END_REF][START_REF] Spielmeyer | Occurrence and fate of antibiotics in manure during manure treatments: A short review[END_REF]. To our knowledge, no studies focused on ATC and ACTC fate during anaerobic digestion. While Urb III anaerobic digestion had no significant impact on the removals of tetracyclines, DOX and TC accumulated during Urb I anaerobic digestion (185-692%). Such accumulation was already observed for TC (180%) and CTC-ECTC (1600%) during industrial-scale swine manure anaerobic digestion (Liu et al., 2018). For some OMPs, a high variability in process input and output contents could partly explain this result, given our "one day" sampling strategy. Actually, Mailler et al. ( 2017) observed moderate time variability, from one to two orders of magnitude over one month for some PPs like CBZ, CIP, NOR and OFL in raw sludge before treatment. OMP extractability also varied along the waste transformation. Although extraction and purification losses and MS matrix effects were assumed to be compensated by adding deuterated-labelled compounds (2.3.2.), the LOQs were impacted by the variations in extractability. Individual LOQs were identified for each matrix, impacting dissipation rate calculation when the LOQ/2 value was used. During treatment processes, degradation products could be transformed back to their parent form (e.g. DIC, CBZ, ERY; Göbel et al., 2007;[START_REF] Kasprzyk-Hordern | The removal of pharmaceuticals, personal care products, endocrine disruptors and illicit drugs during wastewater treatment and its impact on the quality of receiving waters[END_REF] and desorption of OMPs from particulate matter could also cause an accumulation over time [START_REF] Köck-Schulmeyer | Occurrence and behavior of pesticides in wastewater treatment plants and their environmental impact[END_REF].

TMP dissipated at high rates when present in urban and territorial substrates, as previously seen [START_REF] Spielmeyer | Elimination patterns of worldwide used sulfonamides and tetracyclines during anaerobic fermentation[END_REF][START_REF] Mohring | Degradation and elimination of various sulfonamides during anaerobic fermentation: A promising step on the way to sustainable pharmacy?[END_REF][START_REF] Feng | Removal of antibiotics during the anaerobic digestion of pig manure[END_REF]. TYL mostly disappeared (>-70%) regardless of the substrate origin in accordance with [START_REF] Withey | Depletion of hormones and antimicrobials in cattle manure using thermophilic anaerobic digestion[END_REF], [START_REF] Mitchell | The effects of the antibiotics ampicillin, florfenicol, sulfamethazine, and tylosin on biogas production and their degradation efficiency during anaerobic digestion[END_REF], [START_REF] Kolz | Degradation and Metabolite Production of Tylosin in Anaerobic and Aerobic Swine-Manure Lagoons[END_REF]. Even if results were semi-quantitative and had to be taken with cautions, SPI was removed from Urb I and Terri II (not shown in Figure 2) as observed by [START_REF] Zhu | Hydroxylation and hydrolysis: Two main metabolic ways of spiramycin I in anaerobic digestion[END_REF] for sewage sludge. [START_REF] Minamiyama | Fate of nonylphenol polyethoxylates and nonylphenoxy acetic acids in an anaerobic digestion process for sewage sludge treatment[END_REF]. In all anaerobic digestion processes, no apparent NP degradation was evidenced with even negative rates in Urb I (-56%) and Agri IV (-41%) processes, illustrating NP accumulation was probably due to NP1EO transformation [START_REF] Ahel | Behaviour of alkylphenol polyethoxylate surfactants in the aquatic environment-II. Occurrence and transformation in rivers[END_REF][START_REF] Lu | Anaerobic degradation behavior of nonylphenol polyethoxylates in sludge[END_REF][START_REF] Murdoch | Biotransformation of Nonylphenol Diethoxylate in anaerobic digesters: Accumulation of metabolites and their effects on digester performance[END_REF][START_REF] Janex-Habibi | Reduction of endocrine disruptor emissions in the environment: The benefit of wastewater treatment[END_REF]. During Urb III and Terri I-II-III anaerobic digestion, NP1EO was removed with no NP accumulation, reflecting a possible simultaneous removal observed by [START_REF] Patureau | Impact of sewage sludge treatment processes on the removal of the endocrine disrupters nonylphenol ethoxylates[END_REF] and [START_REF] Paterakis | The effectiveness of anaerobic digestion in removing estrogens and nonylphenol ethoxylates[END_REF].

PAH dissipation mostly occurred on urban and territorial sites having high inputs but not on agricultural sites. Low molecular weight PAHs were more dissipated than high molecular weight ones, like in [START_REF] Chang | Anaerobic degradation of polycyclic aromatic hydrocarbons in sludge[END_REF]. The 6 aromatic-cycle PAHs, Benzo(g,h,i)Perylene (BPE) and Indeno(1,2,3-cd)Pyrene (IND), were unaffected on all sites and even accumulated. These low removal rates observed on industrial plants are in contradiction with other data from lab-scale anaerobic digestion experiments with spiked sludge [START_REF] Barret | Influence of feed characteristics on the removal of micropollutants during the anaerobic digestion of contaminated sludge[END_REF], more controlled process conditions and homogeneous samples. Accumulation occurred during Urb I and Terri II-III anaerobic digestion for half of the quantified PAHs with no simple explanation based on site process parameters. As already stated for PPs, our one-day sampling strategy may have hindered process efficiency even though for more persistent compounds like PAHs and NPs the time variability of input sludge concentrations is much lower [START_REF] Mailler | Fate of emerging and priority micropollutants during the sewage sludge treatment: Case study of Paris conurbation. Part 1: Contamination of the different types of sewage sludge[END_REF].

Differences between mesophilic and thermophilic anaerobic digestion processes could not be assessed due to low OMP detection frequencies in Agri II samples (thermophilic anaerobic digestion).

There seems to be no global influence of the substrate type on the OMP fate during anaerobic digestion, trends more relying on individual compounds as shown before. Many PPs were not detected or not quantified in input and/or output samples (Table S6, SI for input samples; Table S7 for output samples), limiting the calculation of removal rates. Low OMP concentrations are more

Dewatering

Dewatering processes after anaerobic digestion differed among the sites. The comparison of volatile solid (VS)/total solid (TS) content ratios before and after dewatering (Table S5) allowed assessing if any VS loss occurred [START_REF] Guerra | Occurrence and fate of trace contaminants during aerobic and anaerobic sludge digestion and dewatering[END_REF]. Ratios were significantly identical (Student's t-test), except for Terri II and Urb I processes respectively by screw or filter-press: even if the TS concentration factor seemed correct, dewatering was improper, keeping many solids in the liquid phase. [START_REF] Drosg | Nutrient Recovery by Biogas Digestate Processing[END_REF] confirmed a lower dewatering efficiency by screw-press than by centrifuge.

Organic matter (or VS) loss in the liquid phase may imply a potential loss of OMPs, especially those with a high Log Kow or with ionic charges preferentially sorbed to organic matter.

A dewatering dissipation rate was calculated from the OMP concentrations in raw matter before dewatering and after in the dewatered solid. OMP dissipation could happen if: a) a pollutant either soluble or sorbed to dissolved and colloidal matter was present in the dewatering liquors, b) suspended solids and potential OMPs migrated to the liquors in case of dewatering inefficiency, or c) some polymers added during dewatering changed the interactions between some pollutants and matter making them more "soluble". In the absence of dissipation, OMPs stayed sorbed on the solid phase. Accumulation may be explained by heterogeneous sampling. On Terri II and Urb I sites with low dewatering efficiency, OMPs with high affinity to suspended solids like PAHs, FLX, CBZ, TRI, For the 3 centrifugation processes (Agri I, Terri I, Urb III), very little dissipation occurred, e.g.

for CBZ, DIC, NP, some PAHs especially in Urb III, and accumulation was observed for NP1EO and some PAHs. The role of centrifugation in the OMP fate is also not well documented. [START_REF] Mailler | Priority and emerging pollutants in sewage sludge and fate during sludge treatment[END_REF] reported no significant dissipation of PAHs, NP and NP1EO during sludge centrifugation. Other compounds like TMP, macrolides, fluoroquinolones, IBU, GEM, TRC were rather unaffected by centrifugation whatever the process.

Liming

The liming process followed anaerobic digestion and thermal dewatering processes (Urban III). The resulting CaO-sludge mixture was compacted into land-spreadable pellets. Liming increased pH mixture from 7 to >12, decreased water content through the addition of CaO and the resulting exothermic reaction, creating unsuitable conditions for microorganisms and stabilising waste matrix.

Dissipation occurred for DOX, TC, TMP, FLX, CBZ, TRI and low molecular weight PAHs. High molecular weight PAHs saw either no changes or accumulated during the liming process.

Accumulation also occurred for NOR and OFL. Given the short time of treatment and its additive nature, concentration changes were only due to physicochemical phenomena in line with the pH increase and the exothermic reaction, inhibiting biological reactions and potentially modifying the interactions between OMPs and their bearing phases. Indeed, pH increase may solubilise organic matter and thus change OMP solubility and extractability from the matrix, resulting in overall concentration increase, i.e. for PAHs, NOR, OFL. For positively-(CBZ) or negatively-charged OMPs at pH 12, strongest interactions may occur through cation exchange and bridging with added Ca 2+ , reducing extractability interpreted as apparent dissipation as supposed by [START_REF] Ogunyoku | Removal of Triclocarban and Triclosan during Municipal Biosolid Production[END_REF] for the increase of TRI concentration during liming. Changes in sorption strength could also occur with pH changes.

Composting

Quinolone and fluoroquinolones were highly dissipated during composting on Urb sites. [START_REF] Haiba | Fluoroquinolones and sulfonamides in sewage sludge compost and their uptake from soil into food plants[END_REF] and [START_REF] Lillenberg | Presence of fluoroquinolones and sulfonamides in urban sewage sludge and their degradation as a result of composting[END_REF] found similar results for NOR, CIP and OFL with reduction rates up to 95%. FLQ concentration sharply decreased in Urb II, which was not reported before to the best of our knowledge. Agri composting diminished ENR contents. Liu (2018) found a removal rate of about 80% for ENR when composting swine manure. Biotransformation could be the main reason behind dissipation. [START_REF] Maia | Degradation of fluoroquinolone antibiotics and identification of metabolites/transformation products by liquid chromatography-tandem mass spectrometry[END_REF] showed high bacterial biodegradation under aerobic conditions for OFL, NOR, CIP and Prieto et al. ( 2011) over 90% decrease for CIP and NOR with white-rot fungus (T. versicolor).

Tetracyclines were also dissipated at high rates during composting in both urban and agricultural settings, either after anaerobic digestion (Urb I, Agri I) or not, in coherence with published rates: 74%, 92%, and 70% for CTC-ECTC, OTC and TC when composting manure [START_REF] Wu | The behavior of tetracyclines and their degradation products during swine manure composting[END_REF][START_REF] Massé | Potential of biological processes to eliminate antibiotics in livestock manure: An overview[END_REF]; up to 35% removal for TC when composting digested sludge [START_REF] Khadra | Fate of antibiotics present in a primary sludge of WWTP during their co-composting with palm wastes[END_REF]. Interestingly, lower dissipation rates were obtained on all sites for ACTC and ATC. TC was rapidly transformed into ATC in other contexts (Halling-Sørenson et al., 2002;[START_REF] Jia | Simultaneous determination of tetracyclines and their degradation products in environmental waters by liquid chromatography-electrospray tandem mass spectrometry[END_REF]; this could explain a lower dissipation rate for dehydrated forms, with ATC and ACTC molecules continuously brought by TC and CTC-ECTC transformation.

TMP was only dissipated in Urb II at 100% compared to 35% for sewage sludge cocomposting in [START_REF] Khadra | Fate of antibiotics present in a primary sludge of WWTP during their co-composting with palm wastes[END_REF]. Macrolides highly dissipated (>70%) as previously seen for TYL and ERY (>95%; [START_REF] Cessna | Veterinary antimicrobials in feedlot manure: Dissipation during composting and effects on composting processes[END_REF][START_REF] Ho | Degradation of veterinary antibiotics and hormone during broiler manure composting[END_REF] during composting of cow/broiler manure.

Other PPs, when detected, were strongly dissipated during urban and agricultural composting, except FLX and CBZ that accumulated in Urb II. Globally, Urb I and II had high dissipation rates.

NPs dissipation rates were more site-dependent with medium to high values in Urb I and Agri I and no changes in Urb II. [START_REF] Zheng | Biodegradation of nonylphenol during aerobic composting of sewage sludge under two intermittent aeration treatments in a full-scale plant[END_REF] and [START_REF] Lashermes | Sorption and mineralization of organic pollutants during different stages of composting[END_REF] observed a 50-60% reduction in NP content during sewage sludge composting. No information was available in the literature concerning NP dissipation during manure composting.

Eleven and 12 of the 13 PAHs accumulated during Urb I and II composting, possibly due to non-extractible PAHs desorbed during organic matter degradation (hence freeing previously trapped compounds), bad sampling or atmospheric deposition. For Urb II, the addition of green waste cosubstrate (OMP content not quantified) could also explain this increase. There were no changes in Agri III but ten PAHs (of low to medium molecular weight) were dissipated during Agri I composting, probably due to the 12 week maturation period. According to [START_REF] Amir | Fate of polycyclic aromatic hydrocarbons during composting of lagooning sewage sludge[END_REF], this decrease could stem from both sorption on non-accessible sites in organic material and biodegradation by thermophilic microbial populations. A higher dissipation of smallest PAHs could indicate a preferential degradation by microorganisms whereas biggest compounds, more hydrophobic, could be more easily sorbed on organic matter and less degraded.

Overall, total concentrations of PPs were highly decreased during all composting processes.

Results were contrasted for PAHs: total PAH concentrations are expected to decrease during composting [START_REF] Amir | Fate of polycyclic aromatic hydrocarbons during composting of lagooning sewage sludge[END_REF][START_REF] Ahtiainen | Microbial toxicity tests and chemical analysis as monitoring parameters at composting of creosote-contaminated soil[END_REF] with smallest compounds preferentially degraded but this was only observed in Agri I. Results were more process-dependent for NPs with reduction only observed when composting anaerobically digested inputs.

The combination of anaerobic digestion and composting was also evaluated in Agri I and Urb I. This combination is common to stabilize organic waste depending on the final uses. In this case, OMP dissipation rates were established considering the input and output concentrations of the combined processes, normalised with the ash content (2.4.4.). For all pollutant types, both sites were significantly more efficient in dissipating OMPs, than single processes (Figure 2, "Combined": dissipation rate from anaerobic digestion input to composting output integrating dewatering).

Considering Urb I and Agri I together, tetracyclines were more dissipated by post-anaerobic digestion composting than by only anaerobic digestion. ACTC and ATC were mainly dissipated during Anaerobic digestion and composting had similar dissipation efficiencies for PAHs and NPs on both sites. NPs when detected were highly dissipated by combined processes. Process efficiency did not seem to be linked to initial OMP amount.

This dissipation improvement may be explained by the combination of process conditions:

bacterial consortia are fully different; the switch from a reductive environment to an oxidative one allows for different degradative pathways. Anaerobic digestion stabilises the organic matter matrix as well as reduces particle size, releasing some OMPs that can be dissipated during composting or increasing interaction surfaces. It would be interesting to compare the effect of composting alone, anaerobic digestion and anaerobic digestion + composting on the same substrate in parallel to decipher more specifically the role of each system.

Conclusions

In situ quantification of 53 OMPs in 10 industrial OW treatment lines was performed. A huge diversity of pollutants was detected in processes input samples according to OMP uses and OW types, at concentrations similar to those found in literature. Less studied OWs, territorial mixes, revealed an intermediary OMP composition, between urban and agricultural settings. For dewatering processes, particularly those with the lowest efficiency, either soluble and charged (tetracyclines) or hydrophobic (FLX, PAHs) OMPs could be released in the aqueous fraction which is thus important to consider when (i) calculating mass balance on the overall treatment line and (ii) assessing the impact of such aqueous fraction if used as fertilizer. Some OMPs like PAHs and DIC were dissipated during thermal treatment due to either volatilization or temperature sensibility. During liming, either dissipation (e.g. DOX, TC, CBZ, TMP, TRI, FLU to PYR) or increase of concentration (e.g. NOR, OFL, DBA, BAP) were observed due to the drastic change in pH, moisture and temperature, modifying the interactions between OMPs and organic matter. Anaerobic digestion had positive effect mainly on fluoroquinolones, macrolides, TMP, DOX, ACTC, ATC and NP1EO whereas composting was more effective on all studied OMPs (except PAHs). Combination of processes enhanced most OMP dissipation. Overall, dissipation was mostly affected by process type and more compound specific behaviour was observed. Waste origin had no effect on dissipation.

These results are general trends of dissipation for a large OMP diversity and for 8 anaerobic digestion, 6 dewatering, 1 liming, 4 composting and 2 combined anaerobic digestion + composting real-scale treatments. Preference was given to the number of processes studied, rather than just one treatment with its temporal variability and sludge retention time. However, this complete OW treatment line approach brings in situ data that can be used for building or completing global models of OMP fate during OW treatments, from waste production to field uses, particularly for models of environmental risk assessment of OW spreading.

Investigation of more sites is needed to better understand the role of less used processes (thermophilic anaerobic digestion, liming…) and establish finer trends for dissipation of individual compounds.

Other pharmaceuticals

Figure 2: Heat map of pollutant dissipation rates. nc: non calculable = both input and output contents were not detected or detected but with no available LOQ. "Combined" means the dissipation rate from the beginning of anaerobic digestion till the end of composting. "°" indicates a thermal dewatering.

Table 1: Details on each sampled sites and waste treatment processes: Site name, type of ongoing process, link between processes (PC: process continuity), reactor size, process duration (d=days/w=weeks), substrate input, dry matter (DM) content, dewatering efficiency (* significant loss of volatile solids (VS) during the process; more details in Table S4, SI), volatile matter removal (TS: total solids, AD: Anaerobic digestion, AF= Agri-Food industry, GW = Green Waste).

Finally

  , "other" PPs were only dissipated during Urb I and Urb III anaerobic digestion, dissipation rates in agricultural and territorial settings were either non-calculable, or when present, they saw no changes or accumulation during anaerobic digestion. Low to moderate dissipation was observed for GEM, FLX, CBZ, DIC on Urb I site and IBU on Urb III site, in coherence with Martin et al. (2012; GEM, CBZ, DIC and IBU), Gonzales-Gil et al. (2016; CBZ and IBU), Bergersen et al. (2012; FLX) and Malmborg and Magner (2015; FLX) but contradictory to the one of Gonzales-Gil et al. (2016) for FLX. Low to moderate dissipation occurred for TRI and TRC in Urb sites, in agreement with dissipation rates in Guerra et al. (2015; < 30%). In Terri II and III, there was either no change or an accumulation depending on OMPs. Nonylphenol polyethoxylates can be shortened into NP2EO, NP1EO and NP. Mass balances were difficult to interpret since production and degradation could occur simultaneously. NP1EO concentrations decreased in nearly all sites except Agri I. NP2EO was highly dissipated in only Agri I but accumulated in Agri II and Urb III as a possible result of NPnEO (n>2) shortening into NP2EO (or directly into NP1EO and NP)

  sensitive to temporal variations often observed in process input matrices, further impeding the detection of global trends. All sites combined, 17 molecules (NOR, OFL, CIP, ENR, DOX, ACTC, ATC, TMP, TYL, ERY, NP1EO, NP2EO, PHE, PYR, Benzo(a)Anthracene BAA, Benzo(b)Fluoranthene BBF, Benzo(a)Pyrene BAP) had high dissipation rates (>70%), 9 molecules (TC, FLX, CBZ, DIC, IBU, TRC, Fluorene FLU, Anthracene ANT, Benzo(k)Fluoranthene BKF) had moderate rates (30-70%) and 7 molecules (FLQ, CTC-ECTC, OTC, GEM, TRI, FLO, CHR) had low dissipation rates (0-30%) during anaerobic digestion. Five compounds (NP, Di-Benzo(a,h)Anthracene DBA, BPE, IND) were never dissipated by anaerobic digestion.

  NP1EO and NP (hydrophobic interactions), more soluble OMPs like tetracyclines and ERY were actually dissipated. Comparable amounts of PAHs and PPs per gram of dry matter were found in the liquid and solid phases of Terri II samples (data not shown), reinforcing the second hypothesis, i.e. losses by sorption on particulate matter still present in the dewatering liquors. Urb III° thermal dewatering process dissipated most PAHs, CBZ, DIC, IBU, TRI and TRC. High temperatures (300°C) may increase losses by volatilisation for compounds like PAHs or by chemical alteration. Mailler et al. (2014) observed 10 to 40% losses in PAH concentrations during thermal dewatering, which is consistent with our data and a 10-90% dissipation of NPEO concentrations whereas we observed no significant changes for NP1EO and NP2EO. Tuncal et al. (2011) suggested volatilisation as a dissipation mechanism for PAHs and Veeken and Hamelers (1999), a possible hydrolysis in digestate at high temperature (>250°C for a few minutes). Comparison of OMP dissipation rates for Urb III and Urb III° dewatering processes reveals that PAHs were the most temperature sensitive OMPs.

  Agri I anaerobic digestion and Urb I composting mainly due to their accumulation during anaerobic digestion in Urb I. However, ACTC and ATC concentrations in mature composts (per g DM) were the same on both sites, indicating a complementary effect of processes lowering concentrations even after an accumulation in Urb I. Reaching the same final concentration could indicate a lower accessibility of ACTC and ATC left in composts. Agri I presented more tetracyclines and Urb I more fluoroquinolones, yet both had overall similar contribution of anaerobic digestion and post-anaerobic digestion composting in the dissipation of tetracyclines and fluoroquinolones.

Figure 1 :

 1 Figure1: Pollutant occurrences in process input wastes, according to their quantification or detection, ordered by families. Occurrence in % is the number of non-detection, detection or values >LOQ considering all compounds of a given family for all input samples of one setting. Nd = Non-detected.

  e. 1.7% of total antibiotic human use in France (WHO Report on Surveillance of Antibiotic Consumption, 2018) and

17.9% in animals (ANSES Report on veterinary antibiotics sales, 2019). However, trimethoprim (TMP), used mainly in conjunction with sulfamethoxazole for a synergistic effect, was quantified in Terri III anaerobic digestion, Urb I anaerobic digestion and Urb II composting samples in small quantities, 95-128 µg/kg DM, which is closed to the highest values found by

[START_REF] Göbel | Extraction and determination of sulfonamides, macrolides, and trimethoprim in sewage sludge[END_REF]

for activated sludge.

Acknowledgments

This study was part of the DIGESTATE project, funded by ANR (Agence Nationale de la Recherche, France) under Grant ANR-15-CE34-0003-01. Authors would like to acknowledge ANR and INRAE (Department Agronomy and Environment) for financing the doctoral fellowship of Nicolas Sertillanges. They thank also Maureen Le Bars, Ghislaine Delarue, Jean-Philippe Delgenes, Emmanuel Doelsch and all of the sites' staff of all sampled sites for their help.

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