Glyphosate contamination in European rivers not from herbicide application?

doi:10.21203/rs.3.rs-3917957/v1

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Glyphosate contamination in European rivers not from herbicide application?

https://doi.org/10.21203/rs.3.rs-3917957/v1

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The most widely used herbicide glyphosate contaminates surface waters around the globe. Being toxic to aquatic organisms and a possible carcinogenic, mitigation strategies attempt to reduce river contamination, but their impact is not evaluated. Investigating long-term time series, we discovered that – in contrast to the USA – glyphosate river water concentration patterns in Europe contradict a dominant input from herbicide application. Our large meta-analysis clearly shows that for decades, the main source of glyphosate has been municipal wastewater, visible in the close correlation to concentration patterns of, e.g., pharmaceuticals, rather high and constant loads all over the year and failure of mitigation strategies. We suspect that glyphosate enters European rivers as a transformation product of aminopolyphosphonates, which are used in European but not U.S. detergents.

Earth and environmental sciences/Biogeochemistry

Earth and environmental sciences/Hydrology

Despite intense debates on its carcinogenicity,¹ glyphosate sales are expected to reach 900,000 metric tons worldwide in 2025.² In the USA, almost 130,000 metric tons were used in 2012 in the agricultural sector³ with only 5-10% of the annual sales applied to non-agricultural sites.³^,^4,5Glyphosate and its main transformation product aminomethylphosphonic acid (AMPA) are frequently detected in rivers as well as in wastewater and sewage sludge,^{6,7,8,9,10,11,12} which is critical with regard to its “toxicity to aquatic life with long-lasting effects”.¹³ Glyphosate is commonly perceived to enter rivers via quickflow induced by rain events with loss rates below 1% after agricultural¹⁴^,15 or urban applications.^16,17,18While the importance of urban sources has been discussed,^19,¹²^,¹⁴^,20,21,22 we do not understand the significance of the various sources nor the input pathways of glyphosate and AMPA making it impossible to judge the effectiveness of recent mitigation measures in Europe²³ aimed at reducing surface water contamination. To delineate sources of glyphosate and AMPA in surface waters, we analysed long time series of river water contaminations. The first datasets from Europe (but not from the USA) were already in stark contrast to our expectations and common hypotheses, as concentration patterns strongly resembled those known for wastewater markers and not for agrochemicals, leading us to suspect a yet hidden source for glyphosate. Temporal patterns of glyphosate and AMPA concentrations in rivers and streams in Europe (E) and the USA (U) are shown in Figs. 1 and 2 and Tables S1 and S2, further information is provided in the supplementary material.

2.1 Seasonality of concentrations in river water

The general assumption is that glyphosate and AMPA enter rivers after herbicide application in conjunction with rain events.²⁴ All temporal concentration patterns and mass fluxes in the USA followed this hypothesis, often manifested by sharp concentration peaks, in particular for glyphosate, and the parallel appearance of other urban/agricultural herbicides (Supplementary material S1). This is visible at the South Fork Iowa River (Fig. 1a, site U7) with an agricultural catchment, where sharp concentration peaks of glyphosate and AMPA are observed during application times in summer,²⁵ often in parallel to those of the herbicide metolachlor. Similar patterns were also present for rivers with fully urban catchments (e.g., the Sope Creek in Marietta; Fig. 1b, site U12), demonstrating intensive private and municipal use during the growing season. In general, glyphosate peaks often coincided with peaks in the water discharge of the river (e.g., the Yazoo River; Fig. 1c).

AMPA’s temporal patterns were more diverse among the sampling sites, as expected from its longer half-life in soil.²⁶ Reservoirs of AMPA may form that are mobilized over longer periods of time, explaining its higher detection frequency, visible as broad maxima of elevated concentrations over weeks to months instead of sharp concentration peaks. A strong correlation to other persistent herbicide transformation products was present, for example with dechlorometolachlor²⁷ at the Bogue Phalia and Yazoo River (Fig. 1c, Table S1). Larger catchments with different application times, intense use over months (e.g. nine months for the Bogue Phalia River (U9) and Yazoo River (Fig. 1c, Site U10)²⁵), and enhanced microbial transformation in case of subsurface flow, evoke elevated AMPA concentrations over long times,⁴^,¹¹^,²⁵ also in urban catchments, e.g. Fanno Creek (Table S1, Site U1; see also supplementary material S1.1.) Concentration patterns in the USA differed due to differences in climate, agricultural management practices, contaminant transport processes, and catchment sizes (see Table S1), and clearly followed the hypothesis of herbicide application as the main source of contamination in rivers. As expected, mass fluxes of glyphosate, AMPA, and other herbicides increased with higher discharges (Fig. 3a and Fig. S4) similar to other pesticides.

By contrast, these features were not at all representative of the European data (Fig. 2 and Table S2), where these typical agricultural input patterns were rare (e.g., sites E2, E5, E24 (France), sites E39 (Fig. 2a) and E40 (Sweden), sites E61 and E65 (the Netherlands)). Concentration-time series for most European rivers (Fig. 2b-d, Table S2) showed distinctly different and seasonal patterns for glyphosate and AMPA with low concentrations during winter months, strong increases during March-May, and maxima in September-October when river discharge is low (supplementary material S2.2). Sharp glyphosate peaks were limited to single events (site E53 (Helme; Section S2.3d) and sites E3, E10, E17, E18, E44 and E59). Differences in land use, agricultural management practices, crop types, climate, and transport processes present at the various sampling sites did not noticeably impact the concentration patterns in rivers as they did in the USA. Moreover, European concentration patterns over decades were not consistent with the main glyphosate application times for stubble and pre-sowing treatments in spring and late summer/autumn (supplementary material S3.2), as genetically modified glyphosate-resistant crops are not approved in the EU.²⁸ Even mitigation strategies in Europe to reduce and then to prohibit preharvest glyphosate applications or private use (supplementary material S6) or the full ban of glyphosate in Luxemburg (2021-March 2023, see Fig. 2c and sites E70-73) had no effect on reducing glyphosate and AMPA contaminations in rivers. In fact, concentrations often exceeded the proposed European environmental quality standard of 0.1 µg/L set for surface waters used for drinking water abstraction.²⁹

As a measure to discriminate input sources, we calculated the logarithm of the ratio of AMPA to glyphosate concentrations, log(A:G). In small U.S. catchments and European sites with a pure agricultural catchment, this value often fluctuated around a median of -0.1 to 0.1 over time, as exemplified for sites E39, U3 and U12 in Fig. S1. For larger catchments in the USA and sites where glyphosate is applied intensely over the growing season (e.g., U5 and U10), there is a trend towards higher median values (remaining below 0.5), indicating a higher prevalence of AMPA. By contrast, the log(A:G) ratios of most European sites were dominated by AMPA with values >1 (i.e., AMPA concentrations 10 times higher than glyphosate; e.g., sites E3, E6, E8, E15, E16) and even >1.5 (AMPA concentrations >30 times glyphosate) for sites with larger catchments (e.g., sites E33, E56, E62; see Section S3.1). These findings indicate that a rather constant source must be present for both glyphosate and AMPA in Europe, which is unexpected, as glyphosate-resistant crops are not approved and mitigation measures restrict glyphosate application frequencies (supplementary material S6).

Our meta-analysis provides further evidence of a constant input of glyphosate in Europe, as its concentration patterns were not related to those of other herbicides. Instead, one sees a strong correlation to wastewater tracers such as carbamazepine, phosphate, pain killers, and household chemicals (supplementary material S3.3). An impressive example is that of glyphosate and benzotriazole at site E58 (Table S2; Teltowkanal, Berlin).

A remarkably constant input of glyphosate into European rivers was also demonstrated by the long-term glyphosate mass fluxes (Figs. 3 and S3; Section S3.4). Constant base mass fluxes were present even outside the growing season and during periods of extended droughts (e.g., summers of 2013 and 2018) when mobilization by rain was unlikely (Figs. 3b-f and S3, Section S3.4). Assuming a constant source, glyphosate’s and AMPA’s unexpected seasonal patterns in European rivers might easily be explained by constant mass fluxes from a point source diluted by elevated river discharge during winter times with low evapotranspiration, which is a well-described feature of wastewater-derived micropollutants.³⁰

2.2 Glyphosate and AMPA in wastewater

The most likely constant sources for glyphosate and AMPA are wastewater treatment plants (WWTP), as both compounds were commonly detected in European WWTPs at elevated concentrations throughout the entire year,⁸^,¹² including during dry weather periods (supplementary material S4), well explaining the high mass fluxes in rivers. The dominance of this source over agriculture is also visible by the number of positive detects in Berlin (8% / 35% / 56% for glyphosate and 22% / 55% / 95% for AMPA) in surface waters with no / seasonal / permanent wastewater inputs, respectively (Fig. 4) (wastewater discharge alternates into different rivers during the year). Elevated glyphosate concentrations were detected downstream of other WWTPs (e.g., sites E57 and E58 and supplementary material S2.2). The log(A:G) ratios in receiving rivers seem to reflect ratios in WWTP effluents.⁹^,¹⁰^,31

Differences between USA and European river contamination patterns can be explained by the rare detection of glyphosate in U.S. WWTPs.²²^,32 AMPA was more frequently detected but at concentrations lower than often observed in Europe. Differences in treatment technologies, especially disinfection, are not relevant, as only chlorination³³ but not UV treatment³⁴ (both used extensively for disinfection of treated sewage in the USA³⁵) can eliminate glyphosate. Furthermore, changes in disinfection technology of Denver’s main WWTPs in 2018³⁶ did not impact concentration patterns downstream (Site U4, Fig. 1d, details in supplementary material S1.4), where event-based input patterns were visible despite the high wastewater content of up to 85% over months. WWTPs may receive glyphosate and AMPA by runoff into sewers, but a constant input is not expected from urban applications (municipal, private) or applications along railway tracks;³⁷^,38 see supplementary material S5. Input via diet and urine is too low to significantly impact river contamination (supplementary material S5.3).

Dried sewage sludge had glyphosate concentrations of up to 3 mg/kg, highly correlated with AMPA throughout the year (see Fig. S4), even when the WWTP was connected to a separate sewer system, hardly receiving surface runoff from rain events but mainly domestic wastewater.¹⁰High temporal resolution sampling during heavy rainfall in France showed glyphosate and AMPA concentrations to increase simultaneously with those of faecal indicators due to sewer overflow but not with the subsequent concentration peak of agrochemicals.³⁹ Sewer overflow with an increase of wastewater markers may also explain events with elevated glyphosate concentrations in European monitoring data (see events marked with an asterisk in Figs. 3d and f). These findings clearly challenge the common hypothesis of urban herbicide applications as the main source of glyphosate in WWTPs.

The importance of urban sources for glyphosate and AMPA has been discussed,¹⁹^,²⁰^,40 especially for the Netherlands.¹¹^,¹² AMPA is also known to be a transformation product of aminopolyphosphonates, which are intensely used in Europe as antiscalants, bleach stabilizers, and corrosion inhibitors in laundry products, in the textile and paper industries, and in cooling circles,⁴¹ which might well explain AMPA’s concentration patterns in Europe. However, a similar source has not been reported for glyphosate.

Our meta-analysis as well as additional information and model calculations shown in the supplemental material explain, why mitigation strategies in Europe were not successful in reducing glyphosate contamination in rivers. All data clearly indicate the presence of a yet unknown but significant urban source for glyphosate in Europe related not to herbicide application but rather to wastewater - the major indications being that, 1) in contrast to the USA, seasonal patterns in Europe are not consistent with a dominant input from agricultural or urban herbicide applications (supplementary material S5). 2) Constant base mass fluxes of glyphosate are present even during long dry summer periods (e.g., 2013 and 2018) and outside the application period of herbicides (Fig. 3 and S5). 3) Glyphosate and AMPA are detected in WWTPs connected to separate sewer systems receiving mainly domestic wastewater and during dry weather periods³¹ (supplementary material 2.2, Fig. S4). Mass balances indicate a dominant input of glyphosate via WWTPs (supplementary material S4). 4) High loads from WWTPs are not associated with urban areas hypothetically treated with glyphosate when considering reported loss rates after application and WWTP elimination rates, (supplementary material S2.3d). 5) Sales numbers for non-occupational glyphosate use in Germany from 2021 can be estimated to yield WWTP effluent concentrations of 0.008 µg/L, which is much lower than field data (supplementary material S6). 6) Mitigation strategies and even a total glyphosate ban in Luxemburg did not change surface water concentrations or patterns. 7) Concentration patterns of AMPA and glyphosate are very similar, which is unexpected given the two different input pathways for AMPA via surface runoff (from glyphosate) and municipal wastewater (from aminopolyphosphonates).

What might this hidden, as yet unknown source for glyphosate be? Our results reveal the following criteria: 1) A discharge into watercourses via WWTPs; 2) An origin in municipal and household wastewater (supplementary material 2.2); 3) A relevance to the food industry (supplementary Material S2.3); 4) An application/usage over the entire year; 5) An application/usage in most (Western) European countries but not in the USA; 6) A source for both glyphosate and AMPA; and 7) Relevance since at least 1999 (see site E49, Selz at Ingelheim).

We are not aware of any technical or domestic glyphosate applications evoking a constant input into wastewater and rivers leading to a rather constant log(A:G). Instead, we raise the hypothesis that both glyphosate and AMPA are formed from a common precursor used in households. Our ongoing work addresses the role of aminopolyphosphonates used in laundry products as potential sources not only for AMPA but also for glyphosate in Europe.

Acknowledgements

We kindly thank all institutions providing surface water data, site-specific information, and intense, fruitful discussions: Berliner Wasserbetriebe, Thüringer Landesamt für Umwelt, Bergbau und Natur, Hessisches Landesamt für Naturschutz, Umwelt und Geologie, Landesanstalt für Umwelt Baden-Württemberg, Landesamt für Umwelt Rheinland-Pfalz, Landesamt für Umwelt Bayern, Pflanzenschutzamt Berlin, Senatsverwaltung für Mobilität, Verkehr, Klimaschutz und Umwelt, Berlin, Sveriges lantbruksuniversitet and Swedish University of Agricultural Sciences, and Le Gouvernement du Grand-Duché de Luxembourg,Administration de la gestion de l’eau. We also thank the providers of data repositories in North Rhine-Westphalia (DE), France, USA, the Netherlands, Italy (Toscana), and the United Kingdom. We thank Marsha Bundman for editing.

Author contributions

Carolin Huhn developed the hypothesis of wastewater input of glyphosate inspired by our sediment core data analysed by Benedikt Wimmer. Together with Wolfgang Schulz, she organized the data collection for the meta-analysis. Carolin Huhn conducted most of the investigations on agricultural land use, informational aspects of selected sites, and management practices. She screened all data and made the selections included in this manuscript, which she prepared. Lisa Engelbart and Sarah Bieger aided in preparing the figures and took part in literature searches. Marc Schwientek contributed to the catchment-specific interpretation of concentration time series and, aided by Hermann Rügner, supported the data interpretation (e.g., by calculating cumulative mass fluxes and by identifying discharge-related seasonal patterns. They both contributed to intense discussions throughout the study. Wolfgang Schulz supported the work with his expertise in markers for wastewater and agriculture. Stefan Haderlein critically considered all findings of the study and intensely edited the manuscript. All authors were active in improving the manuscript with discussions, further information, and editing.

Competing interest declaration: The authors have no competing interests.

Data availability statement: The headers for Tables S1 and S2 provide information on all data sources used. A large share of the data is available online, some data sets can be provided upon request by the different institutions.

Supplementary information: Supplementary Information is available online, and provides an intense discussion of the surface water data, including additional information regarding all aspects of the meta-analysis as well as further figures supporting our hypothesis.

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There is NO Competing Interest.

NatureWaterHuhn3TableS1USA.pdf
Table S1: Summary of all river water data for glyphosate and AMPA, discharge, and further agrochemicals or their transformation products for sites in the USA, site descriptions, and data sources.
NatureWaterHuhn4TableS2Europe.pdf
Table S2: Summary of all river water data for glyphosate and AMPA, discharge, further herbicides or their transformation products, pharmaceuticals, and household chemicals for sites in Europe (FR, SE, DE, NL, IT, UK, LUX), site descriptions, and data sources.
NatureWaterHuhn5SIdetaileddiscussionandinformation.pdf

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Glyphosate contamination in European rivers not from herbicide application?

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