Plant protection products, pharmaceuticals and … Pesticides...1 Plant protection products, pharmaceuticals and household products in the aquatic environment Emission roadmaps and

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Plant protection products, pharmaceuticals and household

products in the aquatic environment

Emission roadmaps and decentralized measures

Report prepared for TAPES: Input to the Decision Support System

Judith Muis, TU Delft

September 2015, the Netherlands

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Preface

This report focuses on the decentralized measures that can be to used reduce emissions of plant

protection products, pharmaceuticals and household products to surface and (to a lesser extent) ground water. Insight will be provided into via which routes and at which locations the various emerging substances enter the water cycle. This will be represented in an “emission roadmap”. The information from this report will serve as input to the decision support system on emerging substances developed within the TAPES project.

The TAPES-project was initiated by TZW Karlsruhe Germany, The Watergroep (previously Vlaamse

Maatschappij voor Watervoorziening) Belgium, VITO Belgium, KWR Watercycle Research Institute the Netherlands, Erftverband Germany, Fachhochschule Nordwestschweiz Switzerland, Water Board de Dommel the Netherlands, Waternet the Netherlands and Delft Technical University.

More information about TAPES or the DSS can be obtained from Jan Peter van der Hoek (TU Delft/Waternet): [email protected] / [email protected] Website: www.tapes-interreg.eu

mailto:[email protected]

mailto:[email protected]

http://www.tapes-interreg.eu/

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Summary

The occurrence of anthropogenic substances in surface water is of concern for the public, regulators and producers of drinking water from surface water [Schwarzenbach, Escher et al. 2006]. Emerging substances (ES) are of specific concern since data on occurrence, exposure, toxicity, and risks as well as national and international regulatory frameworks to regulate these substances are lacking [Houtman, 2010]. Water authorities and water companies struggle with the question if, where and how to reduce the number and concentrations of these substances in the water cycle. Therefore, the Interreg IV-B project TAPES (Transnational Action Program on Emerging Substances) focuses on creating a web based knowledge platform with all relevant information on ES in the water cycle.

This report focuses on the decentralized measures that can be to used reduce emissions of plant

protection products, pharmaceuticals and household products to surface and (to a lesser extent) ground water. Insight will be provided into via which routes and at which locations the various emerging substances enter the water cycle. This will be represented in an “emission roadmap”. The information from this report will serve as input to the decision support system on emerging substances developed within the TAPES project.

Most of the currently known measures for reducing pesticide emission are focused on land-based

cultivation. As much as nine of the ten measures discussed in this report can be effective for reducing pesticide emission from that specific section of the agricultural sector. This makes sense as land-based cultivation is responsible for about 75% of the total pesticide use. Furthermore, most of these measures concern drift-reduction, since about 70% of plant protection products present in the surface water are caused by drift (see section 1.2). To increase awareness at all levels and to achieve active contribution from every stakeholder, the use of environmental yardstick and integrated pest management should be promoted and be implemented as much as possible. If the EU could stimulate this, it would create even more support.

Almost all pharmaceuticals end up in the surface water via WWTP, and residential areas are responsible for at least 80% of the total load arriving at the WWTP. Yet, most measures for reduced emission of pharmaceuticals focus on the producers and suppliers (pharmacist and healthcare institutes), and not on the users. This is probably because producers and suppliers decide which specific pharmaceutical(s) and what dose the patients should get. However, both pharmacists and doctors are currently bound by various prescription guidelines, which limit their freedom of choice. To allow a successful implementation of measures by these stakeholders, the EU could stimulate them by making the rules more stringent in some respects (implementing ERA in market authorization, make take-back schemes mandatory for every pharmacy, and require industry to research green pharmaceuticals), and in some areas less stringent rules (freedom of choice for “greener” medicines using labelling scheme). This may also increase awareness of these stakeholders about this problem and their responsibility.

This does not mean that patients or citizens are not free to contribute to solve the problem. However, first they (also) have to be more aware of this problem, and as a response they can change their behavior in various ways. For example, by being more cautious with regards to using medicines as a first resort, living a healthier life to prevent (more) medicine use, disposing of unused and/or expired medicines in a proper way, and putting pressure on industry and government to achieve concrete solutions. The EU/national government could create more public awareness via campaigns.

Of the emerging substances examined in this study, the least information was found in the area of

household products. This applies to both consumption, occurrence in surface water, and possible

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solutions to reduce emission. When more is known about the occurrence in surface water and the ecological risks (not discussed in this report) of various household products, more awareness should be created among the public to reduce the use of certain harmful household products and hazardous substances could be phased out with the help from public pressure. A successful example of this is the “Beat The Microbead” campaign, as described in section 3.3.1.

For wastewater substances (pharmaceutical and household products) implementing decentralized

collection and treatment of urine or total wastewater from residential areas (and/or hospitals), including installing RSF will help to reduce emissions of all involved substances.

In figure 4.1, all the measures concerning the reduced emission of plant protection products

(green), pharmaceuticals (red) and household products (blue) are summarized. Two measures effects both pharmaceuticals as household products, and one measure effects all three substances (uncolored).

Figure 4.1 Measures for reducing emission of plant protection products, pharmaceuticals and

household products in the aquatic environment before, during and after use. The uncolored measures nr. 1 and 2 effects emission of both pharmaceuticals and household products, and nr. 3 also effects emission of plant protection products.

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In figure 4.2, an emission roadmap is displayed and the measures from figure 4.1 are linked to the different stakeholders/sources. This indicates at which level the measure should be implemented to be effective. Some measures are linked to multiple stakeholders/sources because of their widespread effect, others because implementation at multiple levels will be the most effective or even necessary for succeeding.

Figure 4.2 Emission roadmap with most important stakeholders, sources and emission routes. Green = plant protection products, red = pharmaceuticals, blue = household products. Color intensity and size of the arrows indicate the contribution of that route to the total emission coming from the corresponding source. The numbers correspond to the measures in figure 4.1; and should be implemented at the route, stakeholder or source with which they are linked.

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Main conclusions:

The routes of plant protection products to the aquatic environment are more diverse than those of pharmaceuticals and household products.

The sections of arable farming (land-based cultivation), flower bulbs (open air and greenhouse) and pome and stone fruits are the major consumers of plant protection products. Therefore, measures should focus on these sectors first.

Measures to reduce pesticide emission are mostly focused on the user itself, whereas the measures for pharmaceuticals are more focused on the producer and supplier. This is mainly due to the nature of the substances, but sharing experiences of the different approaches could be useful.

Measures for reducing pharmaceutical emissions at source are less easy to implement because human health is more important than environmental concerns.

When implementing measures to reduce pharmaceutical emissions, the pharmaceutical industry, pharmacists and doctors should be involved, because they decide whether or not a patient gets medication, which type and the dose. Pharmacists and doctors are the key players, since they have contact with the users (patients).

Only little is known about the problem of household products in the environment; therefore, almost no measures for this problem could be found in this study. More research concerning occurrence and ecotoxicology is needed.

EU and/or national governments should focus on creating awareness among professionals and society about environmental pollution due to the use of pharmaceutical, pesticide and household product and point out their responsibilities and/or possibilities for action.

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Index

Preface ................................................................................................................................................ 3

Summary ............................................................................................................................................ 4

Introduction ................................................................................................................................... 10

Chapter 1: Plant protection products .................................................................................... 11 1.1 Different types, consumption data and occurrence in surface water ......................................... 11

1.1.1 Different types of plant protection products ........................................................................... 11 1.1.2 Use of plant protection products ............................................................................................. 13 1.1.3 Occurrence of plant protection products in surface water ...................................................... 14

1.2 Water cycle entry routes and sources .......................................................................................... 15 1.3 Decentralized measures ................................................................................................................ 17

1.3.1 Before use ................................................................................................................................ 17 1.3.2 During use ................................................................................................................................ 19 1.3.3 After use .................................................................................................................................. 21

Chapter 2: Pharmaceuticals ...................................................................................................... 23 2.1 Different types, consumption data and occurrence in surface water ......................................... 23

2.1.1 Different types of pharmaceuticals ......................................................................................... 23 2.1.2 Consumption data of pharmaceuticals ................................................................................... 24 2.1.3 Occurrence of pharmaceuticals in surface water .................................................................... 25



Chapter 3: Household products ............................................................................................... 35 3.1 Different types, consumption data and occurrence in surface water ......................................... 35

3.1.1 Different types of household products .................................................................................... 35 3.1.2 Consumption of household products ....................................................................................... 35 3.1.3 Occurrence of household products in water ............................................................................ 35



Chapter 4: Overview and conclusions ................................................................................... 40

Literature ........................................................................................................................................ 44

Appendix I: Infographic of Integrated Pest Management............................................... 49

Appendix II: Figure of locations for buffers ........................................................................ 50

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Introduction

The occurrence of anthropogenic substances in surface water is of concern for the public, regulators

and producers of drinking water from surface water [Schwarzenbach, Escher et al. 2006]. Emerging substances (ES) are of specific concern since data on occurrence, exposure, toxicity, and risks as well as national and international regulatory frameworks to regulate these substances are lacking [Houtman, 2010]. Water authorities and water companies struggle with the question if, where and how to reduce the number and concentrations of these substances in the water cycle. Different strategies are available, ranging from preventing the compounds entering the water cycle [noPILLS, 2015] to end-of-pipe solutions such as removal of the substances at wastewater- or drinking water treatment plants [Ternes, Meisenheimer et al. 2002; Reungoat, Escher et al. 2012]. However, often the information available is not organized in such a way that water authorities, drinking water companies and decision makers can easily decide which option is most successful and cost efficient in reducing the risk under location- and system-specific conditions. Therefore, the Interreg IV-B project TAPES (Transnational Action Program on Emerging Substances) focuses on creating a web based knowledge platform with all relevant information on ES in the water cycle.

The knowledge collected by the TAPES-project is relevant for end-users such as water authorities,

drinking water companies, wastewater treatment plants (WWTP) operators, national and local governments, the media and the interested public. In the TAPES-project, the different partners are researching the effectiveness with regards to removal of specific ES of the drinking water treatment techniques UV/H2O2, nanofiltration, GAC, affinity adsorption [Bäuerlein et al., 2012], and the wastewater treatment techniques PAC, ozone, retention soil filters, UV (+H2O2), the 1-STEP filter at Waternet and Dissolved Air Flotation (DAF). For more information on the outcome of these studies, see the reports on Action 5 and 6 on the TAPES website (www.tapes-interreg.eu). However since these measures can be very expensive and additionally sometimes not sustainable, it is also interesting to investigate the possible non-technical and/or decentralized measures. Besides the research on treatment technologies also a Decision Support System (DSS) on emerging substances is developed within TAPES. The specific aim of the DSS is to focus on the management of emerging compounds within the whole water cycle, to suggest mitigation methods also beyond technical solutions, make use of the enormous amount of (scientific) information available, while being a simple and easy-to-access tool for the informed but not-expert user, that does not require any particular training. For more information about this DSS see the software and report Action 8 and 9 on the TAPES website.

This report is the result of a literature study on the decentralized measures that can be to used reduce emissions of plant protection products, pharmaceuticals and household products to surface and (to a lesser extent) ground water. Insight will be provided into via which routes and at which locations the various ES enter the water cycle. This will be represented in an “emission roadmap”. This roadmap will be useful for determining the various potential measures. In the research to these measures, the focus will primarily be on possible non-technical, decentralized and/or political measures and these may differ among the various user groups, routes and substances.

Chapter 1 focuses on plant protection products, chapter 2 on pharmaceuticals and chapter 3 on

household products. Every chapter includes consumption data, occurrence in surface water, water cycle entry routes and sources, and decentralized measures. In chapter 4, an overview of all these measures are given and subsequently linked to the different water cycle entry routes in one emission roadmap. At the end, a list of conclusions is provided to finalize the report.

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Chapter 1: Plant protection products

The Netherlands is the largest exporter of agricultural and horticultural products after the United

States. The current intensive and mass production of agriculture makes it necessary to use a large amount of agricultural chemicals, including plant protection products. These substances pose a major risk to the water quality of its many water bodies. A lot of research has been done the past few years regarding to this type of threat. Therefore, the content of this chapter is mainly based on data from Dutch research. The European Union divided the European countries into three different zones based on their environmental conditions, and The Netherlands are in the same zone as Belgium, Germany, the UK and Luxembourg [Snoo and Vijver, 2012]. This means for example that these countries can use the same risk assessment for authorization of plant protection products.

1.1 Different types, consumption data and occurrence in surface water

1.1.1 Different types of plant protection products

In agriculture, different types of plant protection products can be used. According to the Environmental Protection Agency (EPA), there are 19 different groups within which the same pests are addressed [EPA, 2015]. These are listed in table 1.1, together with their effect.

In the TAPES project, a selection of plant protection products was made based on expert group

discussions: Herbicides diuron, mecoprop-p (MCPP), chloridazon, MCPA and AMPA (metabolite of

glyphosate) Insecticide imidacloprid Molluscicide metaldehyde

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Table 1.1 Types of plant protection products and their effects [EPA, 2015].

Type of pesticide Effect

Algicides Control algae in lakes, canals, swimming pools, water tanks, etcetera

Antifouling agents Kill or repel organisms that attach to underwater surfaces, like boat bottoms

Antimicrobials Kill microorganisms (such as bacteria and viruses)

Attractants Attract pests (for example, to lure an insect or rodent to a trap)

Bioplant protection products

Plant protection products from natural materials as animals, plants, bacteria, certain minerals

Biocides Kill microorganisms

Disinfectants and sanitizers Kill or inactivate disease-producing microorganisms on inanimate objects

Fungicides Kill fungi (including blights, mildews, molds, and rusts)

Fumigants Produce gas or vapor intended to destroy pests in buildings or soil

Herbicides Kill weeds and other plants that grow where they are not wanted

Insecticides Kill insects and other arthropods

Miticides Kill mites that feed on plants and animals

Microbial plant protection products

Microorganisms that kill, inhibit, or out compete pests

Molluscicides Kill snails and slugs

Nematicides Kill nematodes (microscopic, worm-like organisms that feed on plant roots)

Ovicides Kill eggs of insects and mites

Pheromones Biochemicals used to disrupt the mating behavior of insects

Reppellents Repel pests, including insects (such as mosquitoes) and birds

Rodenticides Control mice and other rodents

Defoliants Cause leaves or other foliage to drop from a plant, usually to facilitate harvest

Desiccants Promote drying of living tissues, such as unwanted plant tops

Insect growth regulators Disrupt the life processes (molting, maturity and others) of insects

Plant growth regulators Alter the expected growth, flowering, or reproduction rate of plants

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1.1.2 Use of plant protection products

- 70% of the total amount of plant protection products used is used in arable farming (potatoes, corn, etc.), but the use per hectare is >10 times more in bulb cultivation

The Food and Agriculture Organization of the United Nations – Statistics Division (FAOSTAT) is

collecting various statistical data from many countries all over the world, concerning food and agriculture [FAOSTAT, 2015]. Their database also includes data about the use of plant protection products from 1992-2012. The use of plant protection products between 2010 and 2012 in some European countries is shown in table 1.2.

Fungicides & Bactericides Herbicides Insecticides

2010 2011 2012 2010 2011 2012 2010 2011 2012

Austria 1.685 - - 1.589 - - 156 - -

Belgium 1.813 2.354 2.601 1.921 2.483 2.720 606 659 563

France 29.829 - - 22.632 - - 1.033 - -

Germany 9.667 10.088 8.774 16.675 17.913 19.871 1.244 1.109 1.090

Netherlands 3.613 4.239 4.656 2.642 3.025 3.042 1.635 308 304

Norway 84 97 116 574 679 628 5.3 5.9 6.5

Poland 5.360 5.766 5.922 10.489 12.409 12.654 888 973 1.272

Portugal 9.475 9.968 - 2.042 1.995 - 389 345 -

Spain 11.878 10.153 - 10.060 10.891 - 14.335 13.752 -

Sweden 212 213 216 1.687 1.495 1.513 34 33 35

Switzerland 895 922 928 852 871 786 68 80 95

United Kingdom 5.521 5.321 5.787 7.466 7.359 7.835 890 828 672

Table 1.2 Use of plant protection products in different European countries from 2010-2012 [FAOSTAT, 2015].

There is also a widespread difference in plant protection product use between the different agricultural sectors. According to Dutch research, it seems that arable farming (potatoes, corn, cereals etc.) are responsible for about 70% of the total use of plant protection products (see table 1.3). That is mainly because it is the sector with the largest (plant protection product-treated) area. Within arable farming, the use of plant protection products is the highest for cultivation of potatoes. The total use for seed, starch and ware potatoes is 2.276.830 kg/year, which is 61% of the total use per year in arable farming. But when looking at the use per hectare, the sector cultivating flower bulbs and tubers is pointed out as the major consumer. This applies to both greenhouse and open field cultivation.

When looking into the use of plant protection products by Dutch governmental institutions, the

total use in 2009 was 25.379 kg, which is very little compared to the agricultural use [CBS Statline, 2013a]. In 2005 the total governmental use was 53.594 kg, which indicates that there has been a decline of more than 50% in the past few years. Municipalities are responsible for more than 80% of the total governmental use, and they use almost exclusively herbicides (99%; mostly glyphosate).

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Table 1.3 Use of plant protection products in Dutch agriculture per sector during the years 2004, 2008 and 2012 [CBS Statline, 2015].

Pesticide-treated area (x 1.000 ha)

Total use of plant protection products (x 1.000 kg)

Use per hectare (kg/ha)

2004 2008 2012 2004 2008 2012 2004 2008 2012

Arable farming

726 678 649 3.606 3.813 3.754 4.9 5.3 5.5

Vegetables in the open

32 27 28 150 100 130 4.7 3.2 4.1

Pome and stone fruits

17 17 15 490 471 424 29.3 28.1 26.3

Arboricultural crops

14 14 15 110 102 148 7.9 6.9 9.0

Flower bulbs and tubers

20 21 21 933 893 1.140 45.7 41.9 54.4

Greenhouse vegetables

3 4 4 40 45 47 12.3 12.3 12.1

Greenhouse flowers

4 4 3 123 123 129 28.9 32.6 37.9

Mushrooms

0.07 0.02 0.007 2 0.3 0.002 20.2 4.3 0.3

Total 817 764 735 5.454 5.546 5.772 6.6 6.9 7.4

1.1.3 Occurrence of plant protection products in surface water

Plant protection products end up in the surrounding environment via spray drift, leaching and evaporation. To what extent this occurs is determined by the application method, composition of the product, sprayed quantities, speed of the tractor, nozzles etc., but also weather conditions such as wind speed and direction, the crop size and type of soil. Especially the small waters, directly connected with the agricultural parcel, are vulnerable. Besides, plant protection products can also be a risk for the people who apply the plant protection products or who live near a treated parcel. At last, it can also create a risk to recreational users on or in the polluted water [Snoo and Vijver, 2012]

Not many publications were found which included pesticide concentrations in surface waters in

Europe. However, a Dutch database containing concentrations in Dutch surface waters called “Bestrijdingsmiddelenatlas” (plant protection product atlas) exists. The average concentrations and the long term trends of the selected plant protection products for TAPES found in this database are listed in

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table 1.4 [Bestrijdingsmiddelenatlas, 2015]. For a few plant protection products it is clear that the average concentration is declining throughout the years, namely: diuron, MCPP and metaldehyde. Imidacloprid is also declining but not with a constant factor. Chloridazon reached its lowest level in 2006, after which its concentration slightly increased in the following years. The concentrations of MCPA fluctuated between 38 ng/l - 54 ng/l (with one peak in 2009) between 1997 and 2013, without a clear downward trend. This also applies to AMPA, only within a bigger range (85 ng/l - 258 ng/l) [Bestrijdingsmiddelenatlas, 2015].

This is not representative for other European countries, but concentrations of several plant protection products in various countries can also be found in the EMPODAT database, developed and maintained by the NORMAN network (also see section 2.1.3). This database contains occurrence data on emerging substances, including some plant protection products [NORMAN, 2013]. As none of the TAPES substances was included these are not listed here.

Table 1.4 List of selected TAPES plant protection products along with the trends of their concentrations in Dutch surface waters during the years 2003, 2008 and 2013 [Bestrijdingsmiddelenatlas, February 2015].

Pesticide Average concentration in Dutch surface waters (ng/l) *

2003 2008 2013

Diuron 30.3 11.4 6.8

Mecoprop (MCPP) 44.6 33.6 30.1

Imidacloprid 15.6 24.8 15.7

Metaldehyde 102.3 55.6 25.8**

Chloridazon 24.5 13.6 19.0

MCPA 46.5 45.9 37.7

AMPA 276.8 167.3 308.0

* All were above reporting limit ** Data from 2012; no measurement data of 2013 available

1.2 Water cycle entry routes and sources

- 70% of plant protection products present in surface water are caused by drift As already mentioned in section 1.1, the main source for plant protection products in surface water

is agriculture (~5.772.000 kg in 2012). The emission routes from plant protection products use to surface water are illustrated in figure 1.1. The emission from greenhouses differs between land-based (fig. 1.1A) and hydroponic (fig. 1.1B) cultivation [Rijkswaterstaat WVL, 2015a]. For the cultivation of crops in the open air (fig. 1.1C), the emission rates have been estimated using data from an article of the University of Leiden [Snoo and Vijver, 2012]. According to this study, an estimated 70% of the total

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amount of plant protection products present in surface water is caused by drift, 20% by greenhouses and 10% by runoff. These percentages are mainly representative for the Dutch situation.

The contribution of sewage overflows is estimated at about 1% of the load that arrives at the WWTP [Grontmij, 2011; Erftverband, 2015]. This is especially true for combined sewer overflows; loads from separate sewer overflow are much smaller (<0.5%). But for small receiving waters, this route can be more relevant because this flow is not treated.

Figure 1.1 Routes of plant protection products to surface water due to agricultural use. A: land-based cultivation in greenhouses. B: hydroponic cultivation in greenhouses. C: land-based cultivation in open air [Snoo and Vijver, 2012; Rijkswaterstaat WVL, 2015a]

In the Netherlands the government is responsible for only a small amount of plant protection

products (25.379 kg in 2009) [CBS Statline, 2013a]. The routes for plant protection products to surface water due to use for urban maintenance is shown in figure 1.2. Dutch research showed that after use of plant protection products on (semi-)paved surfaces, 60% disappears via sewer into the waste water treatment plant (WWTP), and 40% leaks into the soil and then ends up in surface water via runoff or groundwater [Rijkswaterstaat WVL, 2015b].

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Figure 1.2 Routes of plant protection products to surface water due to governmental use on (semi-) pavements (left side) and unpaved surfaces (right side). A: Governmental use on (semi-)pavements. B: Urban maintenance of (semi-)pavements in residential areas. C: Governmental use on unpaved surfaces within urban areas [Snoo and Vijver, 2012; Rijkswaterstaat, 2014]

1.3 Decentralized measures

1.3.1 Before use

Integrated pest management (IPM) According to the European Crop Protection Association (ECPA) and its member companies, IPM is “a

holistic approach to sustainable agriculture that focuses on managing insects, weeds and diseases through a combination of cultural, biological and chemical measures that are cost effective, environmentally sound and socially acceptable” [ECPA, 2015a]. According to research and full-scale implementation at schools in the United States, it seems that IPM can reduce pest complaints by 78% to 90% without long-term increasing costs, and reduce annual number of pesticide applications by 88% [Gouge et al., 2006; IPM Institute, 2011]. No indication of costs reduction or other savings were found

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for the implementation of IPM in agriculture. The ECPA has created an infographic in which the basics of Integrated Pest Management (IPM) are illustrated. This infographic is included in Appendix I.

Environmental yardstick The Environmental Yardstick for Plant protection products, created by CLM Research and Advice,

provides information on the environmental impact of all crop protection agents permitted on the Dutch market [CLM, 2015]. There are yardsticks for plant protection products for field crops, greenhouse cultivation and municipal authorities, companies and individual citizens. In this way, every plant protection product user is able to compare the different plant protection products and choose a

strategy with a low environmental impact. The yardsticks are available in Dutch and English1.

Crop-free buffer strips Crop-free buffer strips, also called vegetative buffers, can be considered as infrastructure measure

in a catchment [ECPA, 2015b]. These buffers provide infiltration areas for surface run-off water, reduces surface run-off water through appropriate vegetation, they retain sediments, provides habitats that increases biodiversity, and prevents application of plant production products on areas close to surface

water. The USDA2 and CORPEN

3 both recommends buffer width of between 10 m to 20 m for 70-80%

pesticide reduction [ECPA, 2014]. However case studies in the Netherlands show that 4 m could be enough to reduce the emission with 50-89% [Snoo and Vijver, 2012].

According to the authors of the guidance for Best Management Practices (BMPs) for reducing water pollution from run-off and erosion, the right positioning of the buffer in the catchment is usually more important for its efficiency than its width [ECPA, 2015b]. The different locations and their functions are shown in Appendix II. When implementing buffer strips, costs will arise from land being taken out of production and planting, and from establishing and maintaining the buffers [Helmers et al., 2008]. The exact costs depend among others on the type, location and width of the buffers, and on land values.

Underground rain water storage using existing drainage systems Europe is not an arid continent. Yet freshwater scarcity is a concern for almost half of the EU

population [European Union, 2010]. For example, Belgium, Spain and Italy are currently using 20% or more of their long-term supplies every year. A particular measure that can tackle this problem may also contribute to emission reduction: collection of rain water in the underground by using existing drainage systems [Spaarwater, 2015]. This system is currently tested on the Wadden Sea in the Netherlands. Besides testing the system, also the change in run-off of nutrients is quantified. It is expected that the long residence time in the subsoil provides for degradation of rinsed nutrients and plant protection products [Spaarwater, 2015].

Floating cultivation Floating cultivation is an example of a closed water system, a method to reduce pesticide discharge

into the environment in horticulture. The crops are floating in a water system in which nutrients can be added to the water and less plant protection products are needed. In this closed system, all the water is reused [Haan de, 2011].

1 http://www.milieumeetlat.nl/nl/home.html and http://www.milieumeetlat.nl/en/home.html 2 United States Department of Agriculture 3 Comite d’Orientation Pour des Practiques Agricoles Respectueuses de l’Environnement

http://www.milieumeetlat.nl/nl/home.html

http://www.milieumeetlat.nl/en/home.html

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1.3.2 During use

Since drift is responsible for 70% of the amount of plant protection products present in surface

water (see section 1.2), pesticide reducing measures during use are focused on drift reduction. A European Database called Spray Drift Reduction Technology (SDRT) for comparing different drift reducing equipment, reductions and use conditions is currently being prepared by the TOPPS Water Protection project [TOPPS Water Protection, 2015]. There is already a comparison of drift reducing nozzles (50% reduction equipment only for the moment) available for France, Austria, Belgium, The Netherlands and Germany.

Drift nozzles Choosing the right nozzle is very important

for proper spraying and reduction of drift. Which nozzle is most appropriate depends on the driving speed, water quantity, tree height, and required drift reduction [Helpdesk Water, 2015]. At this moment, there are four different categories of drift reduction: 50%, 75%, 90% and 95%. The advantages of this mitigation technique are the low costs (€3-10 per nozzle), the significantly reduced drift and change of currently applied plant protection product is not required [Toolbox Water, 2015]. The disadvantage is that these rough droplet techniques are not effective for some crops. Especially for crops that need smaller droplets, the use of a Wingsprayer is more effective [Helpdesk Water, 2015]

Wingsprayer The Wingsprayer uses air conduction to

spray the small droplets into the crops [Helpdesk Water, 2015]. The downward airflow coming from the wing opens the crops, even while driving. The droplets end up deeper in the crops, which results in a better coverage and therefore a reduced use of plant protection products due to higher efficacy. The price of the Wingsprayer is gross €600/m working width, with a payback period of about 2 to 4 years. The advantages are:

improved infiltration and coverage; reduced use of plant protection products due to higher efficacy (10-30%); 70% to 99% drift reduction; more sprayable days a year; little damage to adjacent parcels or nuisance to neighbors; increased capacity by higher driving speed and less frequently filling of the spray tank; the spray boom is more stable by contact with the crops; the system works by aerodynamics, so fans are not necessary.

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One thing to bear in mind is that this system requires regular manual monitoring of the spray boom height, since a correct height is very important. Another disadvantage is that this system is sensitive to the wind when turning at the headlands. However according to the manufacturer, this effect completely disappeared by the latest developments [Helpdesk Water, 2015].

Air assistance Air assistance on a sprayer causes a downward

airflow, resulting in improved infiltration of the plant protection products into the crops [Helpdesk Water, 2015]. Just like the Wingsprayer, this results in a reduced use of plant protection products (15-30%). Furthermore, the airflow also ensures that the small droplets are less likely to blow away, so the drift is reduced up to 95%. Other advantages of air assistance are more sprayable days per year, capacity increase (requires less water per hectare) and the same result at higher driving speed. On the other hand, incorrect settings may cause more drift and the engine output is higher due to this air assistance system. The calculated additional costs are €20.000-25.000 [Helpdesk Water, 2015]

Drift-reducing additives Drift-reducing additives are agents added to spraying liquid, resulting in a reduced drift-effect

[Helpdesk Water, 2015]. The additives are heavier and bulkier, whereby drift is counteracted. Besides, a drift-reducing additive may also improve on the spray deposition on plant leaves and lower the required dosage. Research shows that at least 20% more plant protection product end up on the leaves when using an additive compared to plant protection products without any additives. The costs for additives can vary from €5-35 per hectare, and it is not always a money-saving measure [Helpdesk Water, 2015]

An example of a drift-reducing

additive is Squall. According to test results, adding Squall improves deposition by 19% to 74%, and reduces drift at least 90% (see picture on the right). Squall also ensures better resistance to rain (no new application after a rain event needed), and moreover, Squall is a biodegradable polymer [Squall, 2015].

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1.3.3 After use

Treatment runoff farmyard According to research in various European countries, the use of plant protection products on the

farmyard and the farmyard itself is contributing about 50-60% of the total load of plant protection products entering the water [CLM, 2014]. For example, after spraying of the crop, the sprayers are rinsed on the farmyard. In most cases, the rinse water is discharged directly into a surrounding ditch. However this rinse water contains high concentrations of plant protection products.

Nowadays there are various systems available for treatment of the rinse water. These systems can

operate on the basis of evaporation and biodegradation [CLM, 2014]. An example is the Phytobac, which is filled with soil and straw of the farmer’s own yard (see figure 1.4A) [Beutech Agro, 2015]. The soil and straw contain bacteria and fungi which can degrade the plant protection products present in the rinse water. Evaporation in the Phytobac takes place by means of solar radiation. Depending on the required capacity, the purchase costs for this system varies between €1.000-€10.000. Another example is the Heliosec, in which 2500 liters of rinse water can be stored (see figure 1.4B) [Syngenta, 2015]. The rinse water evaporates due to wind and sunlight, and the remaining (dry) residue of the plant protection products is left on the plastic sheet. This sheet has to be disposed and replaced at least once a year. The purchase costs for this system are about €5.000.

Figure 1.4 Systems for treatment of runoff from farmyard

A. Phytobac; B. Heliosec [Beutech Agro, 2015; Syngenta, 2015] Prevent discharge of untreated wastewater from the sewers About a third of the used plant protection products in greenhouses ends up in the sewer, and about

60% of the plant protection products used by government on (semi-)pavements do too. Because of leaking sewers and piping and combined sewer overflows (CSOs), untreated water enter the ground- or surface water [Kümmerer, 2010]. To reduce this route of ES, leaking sewers and piping should be repaired and CSOs should be reduced. The first step to reduce CSOs may be to separate the piping systems for wastewater and storm water. Another option is to treat the overflow, so the ES will not end up in the ground- or surface water. Erftverband (Germany) has tested retention soil filters (RSF) downstream of combined sewer overflows, as a possible treatment step by sewer overflows [Christoffels et al., 2014]. In this specific study the removal of pharmaceutical substances (diclofenac

A. B.

22

and ibuprofen) and certain microorganisms, however because of the positive results this also seems promising for removal of plant protection products.

Figure 1.5 Diagram of a Retention Soil Filter [MUNLV, 2003]

23

Chapter 2: Pharmaceuticals

The presence of (residues of) pharmaceuticals in surface water is currently a hot topic in the water sector within the theme of water quality. Many studies have been carried out regarding their presence, the risks and effects in the aquatic environment and the possible measures to reduce their presence [Derksen and ter Laak, 2013]. These studies have revealed that human pharmaceuticals quantitatively by far are the main source of pharmaceuticals into the surface water. Therefore, this chapter focuses only on human pharmaceuticals.


2.1.1 Different types of pharmaceuticals

A pharmaceutical coding system is used to divide pharmaceutical drugs into different groups,

according to the organ or system on which they act and/or their therapeutic and chemical characteristics. This system is called the international Anatomical Therapeutic Chemical (ATC) Classification System. It is managed by the World Health Organization (WHO), and has 5 different levels [WHOCC, 2015]. The first level is a division into fourteen main groups, each with different pharmacological/therapeutic subgroups (second level). The third and fourth levels are chemical/pharmacological/therapeutic subgroups and the last level is the chemical substance. In table 2.1 the fourteen main groups are listed.

Many kinds of pharmaceuticals were detected in the environment during the past years. In the

TAPES project, a selection of pharmaceuticals was made based on expert group discussions, as with the plant protection products:

The anti-inflammatory painkillers diclofenac and ibuprofen (M) The antiepileptic carbamazepine and its metabolite 10,11 transdiolcarbamazepine (N) The bėta-blockers sotalol, metoprolol and metabolite alfahydroxy-metoprolol (C) The antidiabetic metformin and its metabolite guanyl urea (A) The chemical hormone ethinylestradiol (G) The radiocontrast agents diatrizoate (amidotrizoic acid), iopromide, iopamidol and iomeprol

(V) The antibiotic sulfamethoxazole (J)

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Table 2.1 Main groups of the international Anatomical Therapeutic Chemical (ATC) Classification System [WHOCC, 2015]

Code Contents

A Alimentary tract and metabolism

B Blood and blood forming organs

C Cardiovascular system

D Dermatologicals

G Genito-urinary system and sex hormones

H Systemic hormonal preparations, excl. sex hormones, insulins

J Antiinfectives for systemic use

L Antineoplastic and immunomodulating agents

M Musculo-skeletal system

N Nervous system

P Antiparasitic products, insecticides and repellents

R Respiratory system

S Sensory organs

V Various

2.1.2 Consumption data of pharmaceuticals

The consumption of human medicinal products in EU is heterogeneous and varies between 50 and

150 g APIs/capita/year 4 [BIO Intelligence Service, 2013]. France and Germany accounts for approximately two-thirds of this consumption, and although the German population is 25% larger than the French (80 million inhabitants versus 65 millions) the share is an equal split. The UK, Italy and Spain are the second largest consumers with about one-seventh of the consumption each, even though the population of England and Italy (about 60 million inhabitants each), is significantly higher than that of Spain (45 million inhabitants). In term this means that France has the highest consumption per capita of human medicinal products, followed by Germany, Spain, UK, and Italy respectively [BIO Intelligence Service, 2013].

4 API is Active Pharmaceutical Ingredient; the active substance or substance combination of a drug product

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2.1.3 Occurrence of pharmaceuticals in surface water

There are databases with monitoring and/or occurrence data on emerging substances available. One

such database is the EMPODAT Database. This web-based database is developed and maintained by the NORMAN network, which was founded in 2005 with the financial support of the European Commission. The NORMAN network is the European network of reference laboratories, research centers and related organizations for monitoring of emerging environmental substances.

In the EMPODAT database monitoring data from surface water on the four TAPES pharmaceuticals carbamazepine, diclofenac, sulfamethoxazole and metoprolol was found for various European countries. In table 2.2 the average and maximum concentrations (ng/L) of these pharmaceuticals are listed for a selection of European countries, in order to demonstrate the difference in surface water concentrations between the different countries.

Table 2.2 Mean and (maximum) concentration in ng/L of a few pharmaceuticals in river waters of

European countries [NORMAN, 2013].

Carbamazepine Diclofenac Sulfamethoxazole Metoprolol

Belgium (2008-2010)

26 (70) 26 (120) 16 (30) <LoD (<LoD)

France (2006&2012)

28 (510) 19 (60) 13 (81) 24 (70)

Germany (2013)

59 (1200) 92 (1700) 38 (370) 65 (1600)

Italy (2006-2007)

71 (630) 95 (850) 32 (130) n.a.*

The Netherlands (2008-2011)

74 (540) 53 (340) 29 (130) 241 (1180)

Spain (2004-2005)

72 (180) 34 (100) 80 (320) <LoD (<LoD)

Switzerland (2007-2008)

90 (370) 155 (640) 36 (83) 10 (100)

Austria (2007)

52 (150) 2.1 (4.4) 17 (47) n.a.*

*Data not available


In a number of (field)studies, the quantification of pharmaceutical emissions has been further

investigated [STOWA, 2009; STOWA, 2011a; STOWA, 2011b; ter Laak et al., 2013]. From these studies it

26

is clear that in general less than 10% of the total load of pharmaceuticals in surface waters origins from hospitals, other health care facilities contributes with only 1-5%. However, the situation can differ significantly locally, and the contribution to these loads also varies between different pharmaceuticals.

This is also applicable for unused pharmaceuticals. According to a report of the BIO Intelligence Service, the European Federation of Pharmaceutical Industries and Associations (EFPIA) unused humane medicinal products represent 3 to 8% of all the medicinal products sold [BIO Intelligence Service, 2014]. In Sweden, the amount of unused medicines was in 2010 estimated to be about 5%, which correlates with the statement of the EFPIA [Roig, 2010]. In France it was estimated that one out of two prescribed medications is not consumed (i.e. 50% of medicine sold) [Roig, 2010]. However, in both countries, about 5% of the total medicinal products sold are collected or returned to pharmacies [Roig, 2010].

In addition, pharmaceutical waste from health-care activities account, together with other chemicals, for about 3% of the total health-care waste according to the World Health Organization [WHO, 2011].

Figure 2.1 Routes of pharmaceuticals to surface water due to use in medical facilities (A+B) and residential areas [Derksen and ter Laak, 2013; Kümmerer, 2010] A: Hospitals. B: Nursing homes. C: Residential areas. A and B are mostly responsible for only 5-15% of the total load. The blue lines display the disposal of unused medicines.

Rough estimations have been made of the total load of human pharmaceuticals in influent and effluent of the WWTP [Grontmij, 2011]. These estimations are based on measured active substances; immeasurable active substances and degradation products are excluded. The estimated load is 32

27

tons/year (62 ton/year including x-ray contrast media) for influent, and 11 ton/year (24 ton/year including x-ray contrast media) for effluent. The contribution of overflows is estimated at about 1% of the load that arrives at the WWTP [Grontmij, 2011; Erftverband, 2015]. This is especially true for combined sewer; loads stemming from separate sewer overflow are much smaller (<0.5%). But for small receiving waters, this route can be more relevant because this flow isn’t treated.

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2.3.1 Before use

Green pharmacy The term green pharmacy has been defined as “the design of pharmaceutical products and

processes that eliminate or reduce the use and generation of hazardous substances along the whole life cycle” [EEA, 2010]. This covers both the development of more environmentally acceptable and sustainable chemical processes and products (gate to gate approach), and reducing the environmental impact of pharmaceuticals once they have left the industry (gate to grave approach) [Roig, 2010]. So far, only little consideration has been given to this last approach in comparison with the first one. Strategies to prevent pollution and limit the harm of pharmaceuticals on the environment could include:

Reducing the amount of pharmaceutical products at source: minimize therapeutic doses by eliminating exposure to the non-therapeutic isomers (which is also often the cause of unwanted side effects).

Design for biodegradability: designing the pharmaceuticals in a way that they will break down in harmless products at the end of their function and do not persist in the environment.

Although it is very ambitious because the chemical structure is also responsible for its adequate stability and acceptable shelf life, both therapeutic properties and biodegradability of pharmaceutical products can be enhanced by changing the chemical structures [Kümmerer, 2007]. The challenge is to design new drugs that contains a suitable balance between stability and biodegradability. Because of increased externalization of research and the increased pressure to find new drugs nowadays, this is not easy [Snape, 2010]. Moreover, the existing predictive tools may not be good enough yet to be used for development of greener pharmaceuticals in early product development. Besides, there is currently no demand from EU consumers for such green pharmaceuticals, and therefore possibly also no support for associated costs [BIO Intelligence Service, 2013]. Implementation of regulatory incentives to develop active substances with greener characteristics in the current European legislation might be a good stimulation [Kümmerer, 2010; BIO Intelligence Service, 2013].

Better implementation of ERA and requirement at the time of renewal or extension for “old” pharmaceuticals, and for generics lacking an ERA For new authorizations of pharmaceuticals, an Environmental Risk Assessment (ERA) must be

performed (see figure 2.2) and accompany the authorization application according to Directive 2004/27/EC [KNAPPE, 2008]. This Directive came into force on 30 October 2005 [BIO Intelligence Service, 2013]. It involves the generation of data on environmental exposure and ecotoxicity. For medicinal products marketed before 30 October 2005, detailed ERA was not compulsory and was therefore only performed in exceptional cases. Furthermore, no ERA has to be performed for authorization renewals, minor variations and substances like vitamins, proteins, vaccines and herbal products. Also in certain cases, the absence of an ERA will be allowed [BIO Intelligence Service, 2013]

The endpoints of the ERA, when performed and even when published, are hard to find. Although the

Directive 2003/4/EC states: “Member States shall ensure that public authorities are required, in accordance with the provisions of this Directive, to make available environmental information held by or for them to any applicant at his request and without his having to state an interest”, certain exceptions may allow that access to environmental documents is rejected. Especially if this information would

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adversely affect the confidentiality of commercial or industrial information. The European Medicines Agency (EMA) publishes a full scientific assessment report called a European Public Assessment Report (EPAR) for every medicinal product on the European market. However in the related Directives and Regulations, environmental data (including eco-toxicological data) and ERA results are not mentioned as having to be included in the assessment report and/or made publicly available. When EPARs do contain a chapter called Eco-toxicology/Environmental Risk Assessment, this is generally only a brief summary.

In conclusion, improvements can be achieved through better implementation of ERA in the market

authorization and public disclosure of the available environmental and eco-toxicological data. Besides, there are also some deficiencies in the current ERA procedure, questioning its scientific robustness. Key deficiencies of the current ERA framework:

As illustrated in figure 2.2, if the possibility of risk cannot be excluded at the end of the ERA procedure, precautionary and safety measures to limit risk should be performed. However, the environmental impacts are never decisive for approval or rejection of a marketing authorization according to Directive 2004/27/EC [KNAPPE, 2008].

Moreover, using PEC/PNEC ratio for the assessment of risk includes some uncertainties

which limit their relevance. For example, current PNEC values may be based on acute studies when chronic data is not available, and are often based on mortality. In addition, PEC values rely on estimations made in specific environmental conditions, so the variability of conditions that can significantly influence environmental concentrations of pharmaceuticals are usually not taking into account [BIO Intelligence Service, 2013]

The ERA framework also does not consider metabolites or environmental transformation

products in the preliminary exposure assessment, which may represent significant hazard in some cases. And sub-lethal and ecologically important effects related to chronic exposure are not adequately reflected, because the current framework relies on endpoints such as “death”. Therefore, this framework doesn’t seem to be optimal [BIO Intelligence Service, 2013]

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Figure 2.2 Environmental Risk Assessment for human pharmaceutical products [Knappe, 2008] Raising awareness among professionals and public society through information and education Doctors, pharmacists and the public society could be actively involved through information and

education/training to foster changes in behavior [Kümmerer, 2010; BIO Intelligence Service, 2013]. These three categories of stakeholders are priority targets because they are responsible for the prescription, delivery and/or administration/consumption of pharmaceuticals. Environmental considerations could be integrated into medical education and advanced training. Information of the environmental effects of drugs could be introduced in environmental courses and trainings as well, but also as early as in secondary and primary schools. Research shows that information about recycling, given at primary school, influences the parents’ behavior. There is an opportunity to achieve the same effect when informing about pharmaceuticals in the environment [Roig, 2010]. Furthermore, environmental information could be added in packaging leaflets or labelling, with specific precautions relating to the disposal of unused medicines or medicinal waste [Kümmerer, 2010; BIO Intelligence Service, 2013].

Moreover, there are a few successful examples of awareness raising campaigns in France and

Sweden mentioned in the study of BIO Intelligence Service [BIO Intelligence Service, 2013]. In France,

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raising awareness among hospital personnel was brought to the attention in 2009, when a Convection was signed between the Health Ministry and Unions representing hospitals 5. France also had a successful communication campaign about Cyclamed in 2011, which provided information about antibiotic consumption, or more generally, about use of medicines. As a result, 26% more pharmaceutical waste were collected compared to the year before. A similar campaign in Sweden, carried out by Apoteket AB in 2006, resulted in a 12% increase of waste collection [BIO Intelligence Service, 2013]. Sweden also raised awareness by the introduction of a labelling scheme of pharmaceuticals, which is described in the following section.

In addition, other (less prioritized) stakeholders like government authorities, producers,

pharmaceutical committees and environmental/water agencies should be informed. To efficiently reach all the stakeholders involved, both specific and general information should be provided via various communication channels. For these other stakeholders, tailored policy briefs with current issues and best practices could help to gather their support in financing, designing and/or implementing certain measures [BIO Intelligence Service, 2013]

Labelling schemes for pharmaceuticals In Sweden, a classification and labelling schemes of pharmaceuticals is implemented, which targets

specific active pharmaceutical substances [Kümmerer, 2010; Roig, 2010; BIO Intelligence Service, 2013]. It can be used to inform doctors and patients on the environmental impact of the prescribed pharmaceuticals and to create awareness regarding this issue. Because it was not possible to make it mandatory in Sweden due to European rules, the scheme is voluntary [Roig, 2010]. The information on risk/hazard is presented differently for three target groups, with different levels of expertise: patients, prescribers and specialists (scientists, experts etc.). Several developments and refinements to the model are ongoing. It is available on a specific internet portal (www.fass.se), but only in Swedish language.

According to the BIO Intelligence Service, the publication of this scheme did not result in modification of prescriptions as expected, mostly because of the lack of alternative and “greener” medicines. However, it must have increased the overall awareness of the issue, which is also important (see above) [BIO Intelligence Service, 2013].

Reconsidering the appropriateness of packaging sizes for consumer needs Nowadays, medicinal products are usually delivered in standard packaging, not matching the users’

needs. When the marketing authorization holder grants a marketing authorization for forms and packaging of pharmaceuticals which comply with the posology of the user, it would help to prevent unnecessary consumption, extensive costs for the healthcare system and generation of unused medicines [BIO Intelligence Service, 2013]. However, this will probably create costs for marketing authorizations because they may need to change the packaging lines and marketing authorization dossiers.

2.3.2 During use

N.A.

5 More information available at: www.sante.gouv.fr/IMG/pdf/convention-2.pdf

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2.3.3 After use

Take-back schemes of medicinal products Take-back schemes for unused and/or expired medicinal products should be implemented

systematically at every pharmacy. This is one of the simplest ways to reduce the input of pharmaceuticals into the environment [Roig, 2010; BIO Intelligence Service, 2013]. Directive 2004/27/EC requires Member States to “ensure that appropriate collection systems are in place for human medicinal products that are unused or have expired” (Article 1.87). According to a survey carried out in 2007, 19 out of the 27 Member States have a drug take-back scheme in place, but quantitative information on the performance is not easily available for many countries [Taylor and Poulmair, 2007]. Pharmacists’ responsibilities should be clearly outlined and used within collection initiatives, to make sure that implementation and efficiency are increased. In some European countries such as for example France and Norway, contribution to the take-back-scheme is mandatory for every pharmacist [BIO Intelligence Service, 2013]. This scheme is most efficient coupled with public education: when providing patients with information about the importance and efficiency of the collection of unused medicines, it will increase their awareness and change their waste practices [Roig, 2010; BIO Intelligence Service, 2013].

Separate collection of urine by patients Also when the pharmaceuticals are actually used, there is a way to prevent that pharmaceutical residues end up in the sewage: separate collection of the urine and/or feces by the patient itself. The willingness of the patient in order to collect and eliminate their urine was tested in a hospital in Luxembourg (ambulant patients) and Germany (all patients) as part of a European cooperation project noPILLS [noPILLS, 2015]. For two weeks, patients of the radiology department, who received iodinated x-ray contrast media (ICM), were approached to participate in this study. Contrast media represent the biggest load micro-polluting substances in hospital effluent. It is almost entirely excreted in urine in less than 24 hours (50% in 2 hours) after injection, which makes these patients suitable for this study. In Luxembourg, 46% of all ambulant patients (208 in total) were willing to participate and received five urine bags to be used within 24h after getting the ICM injection the patients were also asked to fill out a questionnaire. The urine bags should be disposed in the residual waste after use. Subsequently, 41 patients (43%) returned the questionnaire. These questionnaires showed that 78% of the responders used four or all urine bags and 93% were of the opinion that the urine bags were easy to use. In Germany, 60% of all patients (156 in total) could not participate due to physical or mental conditions. The remaining 40% confirmed their voluntary participation. From the 62 participants, 30% returned the questionnaire. Both studies resulted in a detectable reduction of ICM emissions on hospital and catchment level. They also stated that active involvement of medical staff is a key factor of the separation campaigns, and that these results can be transferred to other substances administered in high amounts in hospitals having similar properties as ICM (excretion path, administration, etc.). However, implementation of separate collection on the level of radiology departments will cost an additional 5 to 10 minutes per patient [noPILLS, 2015].

A similar study was executed in the Netherlands, over a period of 5 months. The goal of this study was not only to get patients to use the urine bag, but also to investigate the willingness of patients to contribute to mitigate this problem [personal contact with Waterboard Groot Salland concerning the project “Getting grip on medicinal residues in our water”, June 25, 2015]. Therefore, the patients were asked to fill in a questionnaire at home, even when they chose not to use the urine bags. This way, the

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reasons why patients did not want to cooperate could also be examined. The questionnaire contained, besides questions about the use of the urine bags, several questions and statements about this issue, responsibilities and possible solutions. The final results are not yet known, but the latest status was that 1228 ambulant patients were approached and approximately 750 patients (~61%) returned the questionnaire 6. The data from these questionnaires are currently being analyzed and will be published in a final report in December 2015.

Separate collection and treatment of urine in residential areas and hospitals Because 80% of the human pharmaceuticals are excreted via urine, separate collection and

treatment of urine could be effective [RIVM, 2012]. Pharmaceuticals will be present in urine at concentrations up to 100 times higher than typical wastewater [Roig, 2010]. Besides, toilets with separate urine collectors use less flushing water, so the urine will be more concentrated. The separated urine flow can be treated at home/hospital location (decentralized treatment) or at the WWTP (centralized treatment). Both approaches are not easy to implement and will cost time and money. In new residential areas it is possible and more cost-efficient to construct a separate system, but if separate systems are only implemented via new construction it will take about 100 years before the whole of the Netherlands has separate systems [Grontmij, 2011]. According to an estimation, separation and decentralized treatment of urine costs about 304 €/m3 of total diluted urine, including investment costs [STOWA, 2010]. Decentralized treatment of urine flow in hospitals are less expensive than in residential areas, due to lower investment costs.

The total load of pharmaceuticals in hospital wastewater is higher than that of residential areas,

except from X-ray agents and anti-diabetic pharmaceuticals [Kumar et al., 2010]. However the relevance of separate treatment of hospital wastewater is still debated, because of the small contribution to the overall environmental load (<10%, see section 2.2) [BIO Intelligence Service, 2013]. In reality it might be more cost-effective because it reduces the need for and costs of end-of-pipe treatments. Furthermore, hospitals may be major contributors if you not only look at loads but at toxicity, considering the significant releases of some specific hazardous molecules such as cytostatics and endocrine therapy drugs. Nevertheless, the contribution of hospitals can differ locally. So, before developing and investing in such a separation systems, the origin, nature and amount of releases from the different sources need to be examined [BIO Intelligence, 2013].

An additional benefit of separating urine flows, is the possibility of feeding the separated urine into

sewer systems in a controlled manner [Roig, 2010]. This is particularly important where sewage and storm water are mixed, because it will be possible to stop discharges of urine during storm events. Therefore, the untreated sewage water, which is normally discharged directly into the surface water during storm events, will be polluted to a lesser extent.

Decentralized collection and treatment of total wastewater streams in residential areas and hospitals Also collection and treatment of the total wastewater streams can be performed. Implementation of

decentralized treatment of hospital wastewater includes adjustments on the (internal) sewer, selection of specific treatment techniques, municipal licenses on the effluent discharge and a guaranteed safety of residents/hospital staff and patients at all times.

When implemented in new residential areas, higher costs on small scale treatment facilities can be compensated by saving money on lower transport costs. An example of a project with cost-efficient

6 Information also temporarily available on www.wgs.nl/gripmagazine (only in Dutch)

http://www.wgs.nl/gripmagazine

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decentralized collection and treatment, is Nieuwe Sanitatie Noorderhoek in Sneek, the Netherlands. Black water (kitchen and toilet, vacuum system) and grey water (washing machine and shower) are separately collected and treated in this residential area. The vacuum system for toilet and sink shredder ensures that there is seven times less water used (cost reduction: €12/p/y). From the black water, biogas can be produced and nutrients recovered. In addition, the grey water can be used for heat recovery (cost reduction: €28/p/y). The total costs of living in this residential area with separated collection, adapted houses and decentralized water treatment are estimated at €400/p/y [STOWA, 2014]

There are also examples of systems where hospital wastewater is collected and treated, such as

Pharmafilter. In this hospital concept, all waste7 is shredded, flushed with water and then disposed into the internal sewer of the hospital [Pharmafilter, 2015]. Together with the rest of the wastewater, it is transported to a treatment plant, designed to remove all hospital specific compounds. This concept also reduces the risk of contamination and improves the working conditions of nurses. About 70% of the effluent water can be reused as process water in the hospital.

In Zwolle (the Netherlands), the water board Groot Salland build a wastewater treatment plant for the hospital ISALA. Different treatment techniques were tested for reducing the pharmaceuticals. The total costs of decentralized treatment of hospital wastewater were calculated to be €4.70/m3 to €5.50/m3 depending on the technique used.8 With these techniques MBR (membrane bioreactor) or MBR combined with UV/H2O2 and GAC (granulated activated carbon), the pharmaceuticals in the wastewater are reduced with less than 50% and over 80% respectively.

Prevent discharge of untreated wastewater from the sewers Due to broken sewers and piping and combined sewer overflows (CSOs), untreated water enters the

ground- or surface water [Kümmerer, 2010]. To reduce this route of pollution, broken sewers and piping should be repaired and CSOs reduced. The first step to reduce CSOs may be to separate the piping systems for wastewater and storm water. Another option is to treat the overflow, so the pollution will not end up in the ground- or surface water. Also for pharmaceuticals retention soil filters (RSF) downstream can be useful (see section 1.3.3) [Christoffels et al., 2014]. About 68% of the RSF inflow samples were positive for diclofenac (max. 1.18 μg/L) and more than 90% for ibuprofen (max. 3.57 μg/L). In the outflow, the maximum concentrations were decreased by 65% for diclofenac and 55% for ibuprofen. The percentage of positive samples at the outflow was reduced to 9% and 17% respectively.

7 They also provide disposable bedpans made of bioplastics, which can be shredded

8 Only MBR (membrane bioreactor) or MBR combined with UV/H2O2 and GAC (granulated activated carbon)

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Chapter 3: Household products


3.1.1 Different types of household products

When discussing household products present in the environment, this may refer to many different substances: fragrances and flavors, softeners, preservatives, UV filters, etcetera. These all originate from care products (like soaps and toothpastes), food, drinks, cleaning products, and clothing, etcetera. For TAPES, three household tracers were selected: the artificial sweeteners sucralose and acesulfame-K, and the antimicrobial disinfectant triclosan.

3.1.2 Consumption of household products

Triclosan is mostly used as a biocide in personal care products (85%), but also in textiles (5%) and plastics and food contact materials (10%). In the year 2006, the consumption in Europe reached 450 tons, and the estimated triclosan production in the EU is 10-1,000 tonnes/year [SCCS, 2010]. Oral metabolism studies showed that 60-80% of the triclosan was excreted in urine, while 12-35% was excreted with feces [Health Canada, 2012].

Artificial sweeteners are mainly used as sugar substitutes in food and beverages, especially for

products used by those who are diabetic and/or obese. Besides this, they are also used in personal care and pharmaceutical products, like toothpastes and pills [Sang, 2014]. In 2006, sucralose was used in more than 4000 products worldwide [Molinary and Quinlan, 2006]. As much as 92% of the ingested amount is excreted unchanged, mostly in feces. Unlike acesulfame, which is excreted mainly unchanged via the renal system [Scheurer, 2009].

3.1.3 Occurrence of household products in water

Due to the widespread use of triclosan, this substance ends up in the wastewater and eventually in surface waters because of incomplete removal by WWTPs. The average removal efficiencies range from 58-99%, depending on the technical capabilities of the WWTPs [SCCS, 2010]. According to various data from worldwide sources (including Europe, USA, Canada, Japan, Hong Kong and Australia), surface water concentrations of triclosan ranged from 0.001-40 μg/L. As for influent, concentrations of 0.002-86 μg/L were found, and in effluent the concentration ranged from 0.002-5.4 μg/L. A study in The Netherlands investigated the concentration of 18 ingredients of household and personal care products in gray water [Leal et al., 2010]. Gray water (kitchen sinks, laundry, hand basins, showers and baths) was collected from a new residential area in Sneek, the Netherlands (see section 2.3.3). In this new residential area, black and gray water are collected separately. The average concentration of triclosan in gray water was

15.66.8 μg/L [Leal et al., 2010]. There have been many discussions about the risk of artificial sweeteners as potential carcinogens

from the beginning of their use, but their use in foodstuff are generally considered to be safe. The concern is nowadays shifted to the ecosystem. Sang et al. established a comprehensive seasonal profile of four types of sweeteners: cyclamate, saccharin, acesulfame and sucralose [Sang et al., 2013]. The last

36

two compounds were found to be much more persistent according to their occurrence data. This is supported by the limited removal for acesulfame (~40%) and sucralose (~20%) found in other studies and >94% removal for saccharin and cyclamate [Loos et al., 2008; Scheurer et al., 2009; Tollefsen et al., 2012].

The concentrations of acesulfame and sucralose have both been measured in several studies in several water compartments. As for sucralose, a screening program in Sweden in 2007 demonstrated concentrations of several μg/L in STP influents and effluents, and also several hundred nanograms per liter in surface waters [Brorström-Lundén et al., 2008]. Tollefsen et al. confirm this in a review: according to the majority of collected data for this review, the maximum effluent concentrations of sucralose were reported to be just below 11 μg/L. Except for two measurements, which were much higher (27 and 119 μg/L, both in USA).

This review also collected data for the concentration ranges of receiving waters and surface waters: 0.004-10 μg/L and 0.001-1.9 μg/L respectively. These findings are supported by an EU-wide monitoring program, which found concentrations up to 1 μg/L sucralose in European surface waters [Loos et al., 2008]. The sweetener was mainly detected in samples from Western Europe and Scandinavia, and less in samples from Germany and Eastern Europe. This means Germany and Eastern Europe likely use other sweeteners.

With regard to acesulfame, the study of Scheurer et al. in Germany showed much higher concentrations in WWTP influent and effluent than for sucralose. The influent concentration of acesulfame in the two investigated German WWTPs ranged from 34 to 50 μg/L, and was discharged at concentrations higher than 20 μg/L into the receiving waters [Scheurer et al., 2009].


No literature was found on the routes and sources of household products. Logically, the route for

these substances will be about 99% via the sewer. The contribution of overflows is expected to be the same as for plant protection products and pharmaceuticals: about 1% of the load that arrives at the WWTP in case of combined sewers [Grontmij, 2011; Erftverband, 2015]. Here too, this route can be more relevant for small receiving waters, because this flow is not treated.

37

Figuur 3.1 Routes of household products to surface water.

N.B. These are estimated percentages, since no literature was found about routes and sources.


3.3.1 Before use

Phasing out hazardous substances in household products The use of hazardous substances in household products can be stopped by campaigns launched by

NGOs. A good example is the campaign “Beat The Microbead” launched in 2012 by the Plastic Soup Foundation together with the North Sea Foundation9. The combined efforts of these NGOs has proven to be very effective: several big manufactures phased microbeads out of their products. This started directly after the campaign launch with six Dutch companies, soon followed by multinational

9 http://www.beatthemicrobead.org/

http://www.beatthemicrobead.org/

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pharmaceutical company Unilever. In 2013, also multinational companies L’Oréal, Colgate/Palmolive, Beiersdorf, Procter & Gamble and Johnson & Johnson pledged to stop the use of microbeads. Subsequently, an international app for smartphones was launched, which allows consumers to check their products for the unwanted presence of microbeads. Nowadays, this app is downloaded more than 100.000 times, and as many as 75 NGOs in 35 countries are supporting Beat the Microbead campaign.

This is a good example of how public pressure can cause phasing out hazardous substances in consumer products.

3.3.2 During use

N.A.

3.3.3 After use

Separate collection and treatment of urine in residential areas This will only be an effective measure for acesulfame and triclosan, and not for sucralose since this

sweetener is mostly excreted in feces (see section 3.1.2). Because toilets with separate urine collectors will use less flushing water, the urine will be more concentrated. The separated urine flow can be treated at home (decentralized treatment) or at the WWTP (centralized treatment). Both approaches are not easy to implement and will costs a lot of time and money. In new residential areas it is possible and more cost-efficient to construct a separate system, but it will then take about 100 years before it is totally implemented in the Netherlands [Grontmij, 2011]. According to an estimation in a study to reduce pollution by pharmaceutical residues, separation and decentralized treatment of urine costs about 304 €/m3 of total diluted urine, including investment costs [STOWA, 2010].

An additional benefit of separating urine flows, is the possibility of feeding the separated urine into

sewer systems in a controlled manner [Roig, 2010]. This is particularly important where sewage and storm water are mixed, because it will be possible to stop discharges of urine during storm events. Therefore, the untreated sewage water, which is normally discharged directly into the surface water during storm events, will be polluted to a lesser extent.

Decentralized collection and treatment of total wastewater streams in residential areas Also collection and treatment of the total wastewater streams can be performed. Implementation of

decentralized treatment of hospital wastewater includes adjustments on the (internal) sewer, selection of specific treatment techniques, municipal licenses on the effluent discharge and a guaranteed safety of residents at all times.

When implemented in new residential areas, higher costs on small scale treatment facilities can be compensated by saving money on lower transport costs. An example of a project with cost-efficient decentralized collection and treatment, is Nieuwe Sanitatie Noorderhoek in Sneek, the Netherlands. Black water (kitchen and toilet, vacuum system) and grey water (washing machine and shower) are separately collected and treated in this residential area. The vacuum system for toilet and sink shredder ensures that there is seven times less water used (cost reduction: €12/p/y). From the black water, biogas can be produced and nutrients can be recovered. In addition, the grey water can be used for heat recovery (cost reduction: €28/p/y). The total costs of living in this residential area with separated collection, adapted houses and decentralized water treatment are estimated at €400/p/y [STOWA, 2014]

39

Prevent discharge of untreated wastewater from the sewers Because of broken sewers and piping and combined sewer overflows (CSOs), untreated water enters

the ground- or surface water [Kümmerer, 2010]. To reduce this route of pollution, broken sewers and piping should be repaired and CSOs must be reduced. The first step to reduce CSOs may be to separate the piping systems for wastewater and storm water. An other option is to treat the overflow, so the pollution will not end up in the ground- or surface water. With respect to this, Erftverband (Germany) tested retention soil filters (RSF) downstream combined sewer overflows [Christoffels et al., 2014]. As already mentioned in section 1.3.3 and section 2.3.3, they tested the removal of pharmaceutical substances (diclofenac and ibuprofen) and microorganisms, but because of the clear positive results this also seems promising for removal of household products.

40

Chapter 4: Overview and conclusions

This chapter first gives an overview of all the measures mentioned in the previous chapters, which

are then linked in an emission roadmap to the source/stakeholder by which it should be implemented. After a brief explanation of this emission roadmap, a number of conclusions are listed to conclude this report.

In figure 4.1, all the measures concerning the reduced emission of plant protection products (green), pharmaceuticals (red) and household products (blue) are summarized. Two measures effects both pharmaceuticals as household products, and one measure effects all three substances (uncolored).

Figure 4.1 Measures for reducing emission of plant protection products, pharmaceuticals and household products in the aquatic environment before, during and after use. The uncolored measures nr. 1 and 2 effects emission of both pharmaceuticals and household products, and nr. 3 also effects emission of plant protection products.

41

In figure 4.2, an emission roadmap is displayed and the measures from figure 4.1 are linked to the different stakeholders/sources. This indicates at which level the measure should be implemented to be effective. Some measures are linked to multiple stakeholders/sources because of their widespread effect, others because implementation at multiple levels will be the most effective or even necessary for succeeding.

Figure 4.2 Emission roadmap with most important stakeholders, sources and emission routes.

Green = plant protection products, red = pharmaceuticals, blue = household products. Color intensity and size of the arrows indicate the contribution of that route to the total emission coming from the corresponding source. The numbers correspond to the measures in figure 4.1; and should be implemented at the route, stakeholder or source with which they are linked.

Most of the currently known measures for reducing pesticide emission are focused on land-based cultivation. As much as nine of the ten measures discussed in this report can be effective for reducing pesticide emission from that specific section of the agricultural sector. This makes sense as land-based

42

cultivation is responsible for about 75% of the total pesticide use. Furthermore, most of these measures concern drift-reduction, since about 70% of plant protection products present in the surface water are caused by drift (see section 1.2). To increase awareness at all levels and to achieve active contribution from every stakeholder, the use of environmental yardstick and integrated pest management should be promoted and be implemented as much as possible. If the EU could stimulate this, it would create even more support.

Almost all pharmaceuticals end up in the surface water via WWTP, and residential areas are responsible for at least 80% of the total load arriving at the WWTP. Yet, most measures for reduced emission of pharmaceuticals focus on the producers and suppliers (pharmacist and healthcare institutes), and not on the users. This is probably because producers and suppliers decide which specific pharmaceutical(s) and what dose the patients should get. However, both pharmacists and doctors are currently bound by various prescription guidelines, which limit their freedom of choice. To allow a successful implementation of measures by these stakeholders, the EU could stimulate them by making the rules more stringent in some respects (implementing ERA in market authorization, make take-back schemes mandatory for every pharmacy, and require industry to research green pharmaceuticals), and in some areas less stringent rules (freedom of choice for “greener” medicines using labelling scheme). This may also increase awareness of these stakeholders about this problem and their responsibility.

This does not mean that patients or citizens are not free to contribute to solve the problem. However, first they (also) have to be more aware of this problem, and as a response they can change their behavior in various ways. For example, by being more cautious with regards to using medicines as a first resort, living a healthier life to prevent (more) medicine use, disposing of unused and/or expired medicines in a proper way, and putting pressure on industry and government to achieve concrete solutions. The EU/national government could create more public awareness via campaigns.

Of the emerging substances examined in this study, the least information was found in the area of

household products. This applies to both consumption, occurrence in surface water, and possible solutions to reduce emission. When more is known about the occurrence in surface water and the ecological risks (not discussed in this report) of various household products, more awareness should be created among the public to reduce the use of certain harmful household products and hazardous substances could be phased out with the help from public pressure. A successful example of this is the “Beat The Microbead” campaign, as described in section 3.3.1.

For wastewater substances (pharmaceutical and household products) implementing decentralized

collection and treatment of urine or total wastewater from residential areas (and/or hospitals), including installing RSF will help to reduce emissions of all involved substances. Conclusions:

The routes of plant protection products to the aquatic environment are more diverse than those of pharmaceuticals and household products.

The sections of arable farming (land-based cultivation), flower bulbs (open air and greenhouse) and pome and stone fruits are the major consumers of plant protection products. Therefore, measures should focus on these sectors first.

Measures to reduce pesticide emission are mostly focused on the user itself, whereas the measures for pharmaceuticals are more focused on the producer and supplier. This is mainly

43

due to the nature of the substances, but sharing experiences of the different approaches could be useful.

Measures for reducing pharmaceutical emissions at source are less easy to implement because human health is more important than environmental concerns.

When implementing measures to reduce pharmaceutical emissions, the pharmaceutical industry, pharmacists and doctors should be involved, because they decide whether or not a patient gets medication, which type and the dose. Pharmacists and doctors are the key players, since they have contact with the users (patients).

Only little is known about the problem of household products in the environment; therefore, almost no measures for this problem could be found in this study. More research concerning occurrence and ecotoxicology is needed.

EU and/or national governments should focus on creating awareness among professionals and society about environmental pollution due to the use of pharmaceutical, pesticide and household product and point out their responsibilities and/or possibilities for action.

44

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Appendix I: Infographic of Integrated Pest Management

[ECPA, 2015a]

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Appendix II: Figure of locations for buffers

1: In-field buffer, used to break up a long slope inside a cultivated field. 2: Edge-of-field buffer zone, protecting a road (potential water pathway). 3: Edge-of-field buffer zone in downslope corner of a field, where water is concentrating. 4: Grassed talweg, to reduce concentrated water flow. 5: Large grassed buffer zone (i.e. meadow), used to intercept, disperse and infiltrate concentrated

water flow exiting from the upslope talweg. 6: Riparian buffer, grassed buffer strip between edge of field and a surface water body, to intercept

diffuse run-off from the upslope field. [ECPA, 2015b]