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CRANFIELD UNIVERSITY Max Bullock Metaldehyde and Its CRANFIELD UNIVERSITY Max Bullock Metaldehyde and its relationship with groundwater contamination and landfill leachate School of Applied Sciences MSc by Research MSc by Research Academic Year: 2013 - 2014 Supervisors: Peter Jarvis and Frédéric Coulon June 2014 CRANFIELD UNIVERSITY School of Applied Sciences MSc by Research MSc by Research Academic Year 2013 - 2014 Max Bullock Metaldehyde and its relationship with groundwater contamination and landfill leachate Supervisors: Peter Jarvis and Frédéric Coulon June 2014 This thesis is submitted in partial fulfilment of the requirements for the degree of MSc by Research © Cranfield University 2014. All rights reserved. No part of this publication may be reproduced without the written permission of the copyright owner. ABSTRACT Increasing attention is directed towards many chemicals and microbial constituents which have not been historically considered as contaminants. These “emerging contaminants” are commonly derived from municipal, agricultural and industrial wastewater sources and pathways. Among others, metaldehyde, a widely used molluscicide, has been detected in groundwater at levels exceeding the 0.1 μg L-1 limit required by the Water Framework Directive. This has raised concerns for drinking water treatment, as the compound cannot be removed with conventional granular activated carbon or ozonation treatment processes. Further to this, some recent case studies on groundwater quality reported metaldehyde concentrations > 0.1 μg L-1 in the vicinity of landfill sites. In all cases, there is no evidence or record of metaldehyde disposal. This growing evidence raises the question about the relationship between the characteristics of leachate generated from the landfill sites, the presence of metaldehyde and its impact on surrounding groundwater resources. In the present study, two landfill sites located in the UK are being investigated as potential sources of contamination to groundwater by metaldehyde. In both cases, metaldehyde concentrations exceeded the levels expected from a point- source contamination site. For this reason, landfill leachate chemistry was assessed to determine whether an in situ synthesis of metaldehyde can occur within landfill sites. A critical review found that potential reagents such as acetaldehyde, catalysts such as acetic acid and environmental conditions are present in groundwater aquifers. However, lab-based experiments have suggested that metaldehyde cannot be synthesised in the environment despite the presence of a wide range of pH values, cold temperatures, a high concentration of acetaldehyde, and the presence of a calcium bromide catalyst. This finding, combined with data i collected from the two case study sites over a 7 month period suggest that a point source of the pollutant is the most likely explanation. The in situ testing also highlighted that the acetaldehyde reagent contained significant contamination by metaldehyde, of which the supplier was unaware. Two independent laboratories also confirmed the presence of metaldehyde in the reagent. Acetaldehyde of a purer grade from other manufacturers was also tested and found to contain significant levels of metaldehyde. These findings demonstrate another potential source of metaldehyde which is not agricultural. Finally, leachate from another UK landfill site was also analysed for metaldehyde to determine how prevalent metaldehyde contamination could be across landfill and was found to be present well above the limit for drinking water. Keywords: Emerging contaminants, In situ synthesis, acetaldehyde contamination, metaldehyde organic mechanism, micropollutants ii ACKNOWLEDGEMENTS First of all, my thanks go to Dr Peter Jarvis and Dr Frédéric Coulon for their continuous support and mentoring during this project. Their shared knowledge and expertise has been of great assistance in helping to steer the direction of this project as new problems and discoveries emerged. For my laboratory work, I would most of all like to thank Catherine Rolph for providing advice on analytical procedures and for helping to solve various problems throughout the project. Great thanks goes to my sponsors, Affinity Water and Anglian Water, for giving me this opportunity for postgraduate study, with particular thanks to Alister Leggatt, Ilias Karapanos, Matthew Rawlinson, Barrie Holden, Mark Berry and Mike Pinchin for their support and great enthusiasm towards this project, which has helped me to get the best out of my abilities. Other people who have helped greatly in this project are Doug Mayer and Leon Warrington (Hydrock), Lothar Ott (Lonza), Pete Simpson and Theresa Cory (Environment Agency) and Ross Goodband (Arcadis). iii TABLE OF CONTENTS ABSTRACT ......................................................................................................... i ACKNOWLEDGEMENTS...................................................................................iii LIST OF FIGURES.............................................................................................vi LIST OF TABLES ............................................................................................. viii 1 Introduction...................................................................................................... 1 2 Aims and objectives ........................................................................................ 2 3 Literature Review ............................................................................................ 3 3.1 Introduction ............................................................................................... 3 3.2 Landfill sites and leachates....................................................................... 6 3.3 Chemical changes in landfill sites and leachate over time ...................... 14 3.4 Metaldehyde ........................................................................................... 17 3.5 In situ metaldehyde synthesis theory...................................................... 18 3.6 Proposed in situ mechanism................................................................... 21 3.7 Sources of reagents................................................................................ 26 3.8 Conclusions ............................................................................................ 27 4 Case Studies – Sites of Investigation ............................................................ 29 4.1 Study Areas ............................................................................................ 29 4.1.1 Helpston ........................................................................................... 29 4.1.2 Smallford .......................................................................................... 31 4.2 Methodology ........................................................................................... 33 4.2.2 Helpston Landfill............................................................................... 33 4.2.3 Smallford landfill............................................................................... 35 4.2.4 Analytical method............................................................................. 36 4.3 Results and discussion ........................................................................... 38 4.3.1 Helpston landfill site ......................................................................... 38 4.3.2 Smallford landfill site ........................................................................ 49 4.4 Other leachates ...................................................................................... 59 4.5 Conclusions ............................................................................................ 59 5 Determination of the feasibility of an in situ synthesis of metaldehyde.......... 61 5.1 Introduction ............................................................................................. 61 5.2 Methodology ........................................................................................... 62 5.3 Results and discussion ........................................................................... 63 5.4 Conclusion .............................................................................................. 68 6 Areas for further research.............................................................................. 70 REFERENCES................................................................................................. 73 v LIST OF FIGURES Figure 1: The major stages of waste degradation ............................................ 16 Figure 2: Formaldehyde and Acetaldehyde...................................................... 22 Figure 3: The reaction of formaldehyde to form the hydrate............................. 22 Figure 4: The reaction of acetaldehyde to form the hydrate ............................. 22 Figure 5: The reaction of the hydrated formaldehyde with itself to form a polymeric chain.......................................................................................... 23 Figure 6: The ring closure reaction of the formaldehyde polymer to form the stable 1, 3, 5 - Trioxane............................................................................. 24 Figure 7: The ring closure reaction of the acetaldehyde polymer to form the stable paraldehyde .................................................................................... 24 Figure 8: The complete proposed organic mechanism for in situ metaldehyde synthesis...................................................................................................
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