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Centre for Environmental Control and Waste Management Department of Civil and Environmental Engineering Centre for Environmental Control and Waste Management Department of Civil and Environmental Engineering http://www.imperial.ac.uk/ewre Sources and Impacts of Past, Current and Future Contamination of Soil Appendix 2 : Organic Contaminants S R Smith and D Riddell-Black JUNE 2007 Dr Stephen R. Smith, Centre for Environmental Control and Waste Management, Department of Civil and Environmental Engineering, Imperial College London, South Kensington Campus, London SW7 2AZ. Tel: +44 (0)20 75946051; Fax +44 (0)20 75941511; Email: [email protected] CONTENTS Note on the report structure and content EXECUTIVE SUMMARY 1 OVERVIEW OF ORGANIC CONTAMINANT INPUTS TO SOIL 1 1.1 Introduction 1 1.2 Persistent organic pollutants 7 1.3 Bulk industrial and domestic compounds 12 1.4 Pesticides 18 1.5 Human pharmaceuticals 20 1.6 Veterinary medicines 25 1.7 Biocides and personal care products 34 1.8 Endocrine disrupting chemicals (EDCs) 34 2 SOURCES OF ORGANIC CONTAMINANTS TO SOIL 39 2.1 Atmospheric 39 2.2 Sewage sludge 48 2.3 Livestock manures 74 2.4 Compost 79 2.5 Other waste materials 91 2.6 Pesticides 96 2.7 Irrigation water 104 3 POTENTIAL IMPACTS ON SOIL, ENVIRONMENT AND HEALTH 110 3.1 Persistent organic pollutants 110 3.2 Pesticides 120 3.3 Veterinary medicines 128 3.4 Di(2-ethylhexyl)phthalate (DEHP) and other phthalates 138 4 SUMMARY AND CONCLUSIONS 150 4.1 Introduction 150 4.2 Sources of OC inputs to soil 150 4.3 Effects of OC inputs on soil quality and function 154 5 RESEARCH RECOMMENDATIONS AND PRIORITIES FOR 159 ORGANIC CONTAMINANTS 6 REFERENCES 163 ANNEXES 181 Note on the report structure and content This report forms an Appendix to the SID 5 Research Project Final Report for Defra Project code SP0547: Sources and Impacts of Past, Current and Future Contamination of Soil. The report here deals specifically with sources of organic inputs to soil and their potential impacts on soil quality, environment and human health. An extensive review of published literature, web information and unpublished reports was completed. The data were organised into three main sections in the report providing: (1) an overview of the identified key groups of organic compounds that may potentially enter soil; (2) a detailed, and as far as possible, quantitative assessment of the extent of the inputs of these contaminant groups from different source pathways; and (3) an assessment of the potential impacts of selected, important groups or specific contaminants on soil, environment and health. The appendices to this report present a list of categries of different compounds, the inventory of reviewed concentration data in environmental media; a list of legislation relating to organic contaminants that has direct or indirect implications for their transfer to soil; a list of chemicals of potential concern for the environment and procedures and legislation relating to pesticides and their approval. EXECUTIVE SUMMARY 1. Introduction Soil is potentially the recipient of inputs of a very large number of organic contaminants (OC). In the past effort has concentrated on examining the fate of OC in the aquatic environment and the potential for direct impact on human health via the food chain. Only more recently has attention focused on the impacts of OC on soil. For the purposes of this report, OC inputs to soils were divided into seven broad groups: • Persistent organic pollutants (POPs); • Bulk chemicals used in industry and domestically; • Pesticides; • Human pharmaceuticals; • Veterinary medicines; • Biocides and personal care products (PeCPs); • Endocrine disrupting chemical (EDCs) 2. Sources of OC inputs to soil Potential sources of OC inputs to soil include: atmospheric deposition, sewage sludge, livestock manure, compost, other ‘wastes’, pesticides and irrigation water. A brief summary is provided below. Atmospheric deposition Information on atmospheric emissions and concentrations of POPs, provides an indirect indication of POP inputs to soils. National emissions data is collected annually in accordance with international treaties to monitor and limit POP emissions. Inevitably, the UK is both a recipient of POPs from overseas and an exporter of emissions. Modelling of long-range transport and deposition of POPs (MSC-E, 2004) has provided reasonable predictions of actual and relative POP concentrations in UK air, soil and vegetation. In general, concentrations have decreased over time and illustrate the effectiveness of action taken during the 1980s and 1990s to curb emissions and reduce the environmental burden of some principal POPs (PCDD/Fs, PCBs and PAHs). There are a variety of routes through which pesticides may enter the atmosphere including spray drift and volatilisation. Since the loss of spray means that chemicals are not being effective it is in the farmers’ interest to minimise losses through appropriate operating practices. The use of aerial application of pesticides has declined substantially in the last 20 years, with applications in 2002 estimated to be equivalent of 0.01% of the total area of pesticide application (CSL, 2003c). Wet deposition is generally the most significant route for pesticide redeposition to soils (Dubus et al., 2000). Sewage sludge. Quality standards for various OC in sewage sludge for agricultural use have been established in a number of European countries. The range of OC with potential health or environmental implications is much greater than the number of PTEs in sludge which are routinely monitored and controlled. Indeed, 42 organic compounds are regularly detected in sludge (IC Consultants, 2001). Many OC will adsorb to the sludge matrix, although a proportion of the volatile OC may be lost by volatilisation during wastewater and sludge treatment. Biodegradation during anaerobic digestion may also eliminate certain OC from sewage sludge, but in general destruction is typically only 15 – 35 %. Aerobic composting and thermophilic digestion processes are generally more effective at OC degradation than mesophilic anaerobic digestion, particularly for industrial bulk chemicals such as the surfactants LAS and NPE. Thermal hydrolysis prior to conventional anaerobic stabilisation may have a significant influence on the removal of OCs from sludge, but the effects have yet to be investigated for this comparatively new treatment process. Controls on POPs introduced between 1980-90 have been relatively effective and there have been significant reductions in the primary sources of PAHs, PCBs and PCDD/Fs (Smith, 2000). This has also lowered inputs to the urban wastewater (UWW) system and reduced concentrations in sewage sludge. Inputs of POPs to sewage sludge now principally reflect: • Background inputs to the sewer from normal dietary sources; • Background inputs by atmospheric deposition due to remobilisation/volatilisation from soil and cycling in the environment (e.g. PCBs, PCDD/Fs and PAHs); • Atmospheric deposition from waste incineration (eg PCDD/Fs); • Atmospheric deposition from domestic combustion of coal; • Biodegradation during sludge treatment; • Volatile solids destruction during sludge treatment. PAHs are Water Framework Directive (WFD) priority hazardous substances and the aim is to cease emissions, discharges and losses of these compounds by 2020 (CEC, 2001). However, curbing the emissions of PAHs and PCDD/Fs from domestic coal burning would be technically difficult and incinerators are already subject to stringent air quality emission standards (EPCEU, 2000a). Consequently, there is probably little opportunity to further reduce the inputs and concentrations of PAHs, PCDD/Fs as well as PCBs in UWW and sewage sludge. POPs generally strongly bind to the sludge solids and the body of scientific evidence suggests that there are no significant environmental consequences from PAHs, PCBs or PCDD/Fs when sludge is applied to agricultural land. In the light of these developments, it may be argued that these substances are no longer as environmentally important as they were. However, soil is a major repository for POPs and further investigations are necessary to improve understanding of the remobilisation and cycling processes that control diffuse inputs of these organic compounds to UWW. Data on the concentrations of pharmaceuticals in materials applied to land is very limited for the UK. In general, studies suggest that the pharmaceuticals vary greatly in biodegradability and are present in sewage influents and effluents to various extents. Typically, 60 % of the compounds in the influent may be removed during wastewater treatment although there is a wide range of removal efficiencies from 7- 99% (Ternes, 1998). Recent investigations show that approximately 90% of potential oestrogenic activity in UWW is reduced by sewage treatment and that <3 % is transferred to the sewage sludge. Oestrogenic substances excreted in farm livestock manures are likely to represent a much greater loading onto soil compared to recycling sewage sludge in agriculture (IC Consultants, 2001). There is concern over persistent pesticide compounds (particularly organochlorines) in sewage sludge due to potential soil accumulation and long-term impacts on the environment (Bowen et al., 2003). Modern pesticides have been developed with improved biodegradabilities in wastewater treatment and in the environment in general, so their presence is less of a concern than in the past. Varying persistences and ecotoxicities have been reported (Boxall et al., 2004). However, the implications for soil quality arise more from direct applications of pesticides
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