The overland transport of veterinary antibiotics Caroline Bailey

161 Pages·2016·9.39 MB·English

The overland transport of veterinary antibiotics

Von der Fakultät für Bauingenieurwesen der Rheinisch-Westfälischen
Technischen Hochschule Aachen zur Erlangung des akademischen Grades
einer Doktorin der Ingenieurwissenschaften genehmigte Dissertation

vorgelegt von

Caroline Bailey

Berichter: Univ.-Prof. Dr.-Ing. Holger Schüttrumpf
Univ.-Prof. Dr. rer. nat. Gerd Hamscher

Tag der mündlichen Prüfung: 18. Dezember 2015

Diese Dissertation ist auf den Internetseiten der Universitätsbibliothek online verfügbar.
This doctoral thesis was initially submitted to the Faculty of Civil Engineering, RWTH Aachen
on 14th October 2015. The public presentation and doctoral examination took place on 18th
December 2015.

Candidate
Caroline Bailey, M.Eng.

Supervisor
Dr. Roy M. Frings

Examination committee
Univ.-Prof. Dr.-Ing. Holger Schüttrumpf
Univ.-Prof. Dr. rer. nat. Gerd Hamscher
Univ.-Prof. Dr.-Ing. Johannes Pinnekamp
Univ.-Prof. i.R. Dr.-Ing. Jürgen Köngeter

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Acknowledgements

The presented work was supported by the German Federal Ministry of Education and Research
(BMBF) and was conducted within the RiSKWa research project Risk AGuA; grant
02WRS1274A.

I would like to thank Professor Holger Schüttrumpf, firstly for offering me employment as a
scientific researcher at the Institute of Hydraulic Engineering and Water Resources Management
(IWW), RWTH Aachen, and secondly for encouraging me to both start and finish this thesis.
Many thanks also go to my supervisor, Dr. Roy M. Frings, for the frequent reviews of thesis
chapters and for the advice offered to me during the process of writing and publishing scientific
papers.

I particularly thank my publication co-authors and Risk AGuA project partners: Professor Gerd
Hamscher and Dr. Astrid Spielmeyer from the Institute of Food Chemistry and Food
Biotechnology (ILL), Justus Liebig University Giessen. It was pleasure to work with you both,
seeing our ideas bought to fruition.

Thanks also go to Professor Wolfgang Dott and his staff from the Institute of Hygiene and
Environmental Medicine (IHU), RWTH Aachen, and Professor Henner Hollert and his staff from
the Institute for Environmental Research (Biology V), RWTH Aachen, for their practical support
and lending of laboratory equipment.

Many people helped me to collect samples: a time-consuming and often dirty task! For this
support I sincerely thank Christian Röder and Frank Wieczorek from the Lower Saxony State
Authority for Mining, Energy and Geology (LBEG); Rita Kramer (Risk AGuA project partner);
Dr. Roy M. Frings and Tobias Schruff (IWW). Particular thanks go to the Höck family for their
long-term co-operation and fantastic hospitality. It was always a pleasure to visit you.

For help with the laboratory experiments, I firstly thank Heinrich Höper from the Lower Saxony
State Authority for Mining, Energy and Geology (LBEG) for providing analyte free lysimeter
water and to Thomas Pütz from the Jülich Research Centre, Germany, for providing an analysis
of both soils that were used. Considerable thanks go to Sarah Nelsen, Darja Reich and Mark
Richert for their practical assistance with the experiments and for the fun I had working with
you.

Many thanks go to Brian Irvine and Mike Kirkby (School of Geography, University of Leeds,
U.K.) for their co-operation regarding the PESERA model. As I began work for this thesis with
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very little programming experience, I am extremely grateful for the days, weeks, and probably
months of my time that were saved by the help offered to me by Tobias Schruff (IWW), Mina
Karamesouti (Agricultural University of Athens, Greece) and especially Filippo Borlenghi.

Personal thanks go to those IWW colleagues and Hiwis who offered me friendship and humour,
despite my sometimes dubious German ability! Sharing a smile with you always improved my
day. Special thanks go to Franziska Ribbe, my Risk AGuA project partner, for her conceptual
and technical advice but mainly for her constant positivity and kindness.

One of the most enjoyable aspects of my role at the IWW was teaching. I thank all the students
whose Bachelor and Master theses contributed knowledge towards this Doctoral thesis, and those
who worked very hard to pass the Hydromechanics course that I helped to teach. I wish all IWW
students the very best of luck with their future studies and careers.

My time in Aachen would not have been the same without some of the fantastic friends I met
along the way! To the girls from the Hermann Straße Wohnheim, the members of both of my
choirs (Sound ‘n’ Soul and AuftACt), the members of Aufwärts Aachen Basketball Club and a
few other special people (Maxi, Heidi, Anne, Hera and Jero, Luisga and Joha): I’m lucky to have
known you. We had some great times!

I thank my family: Graham, Sara and Tom Bailey. They are my constant supporters and the
bedrock of all my successes. I can always rely on them for a photo, message or ridiculous joke to
cheer me up and cheer me on.

And finally, but most importantly, I come to Filippo: my very best friend. Struggling to know
how to express my gratitude to you, I turn to one of our favourite songs:

“But of all these friends and lovers
There is no-one compares with you
And these memories lose their meaning
When I think of love as something new.

Though I know I'll never lose affection
For people and things that went before
I know I'll often stop and think about them
In my life, I love you more.”

Lennon and McCartney
In My Life, Rubber Soul

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Contents
Abbreviations ................................................................................................................................ 9(cid:3)
Symbols ........................................................................................................................................ 11(cid:3)
Figures .......................................................................................................................................... 13(cid:3)
Tables ........................................................................................................................................... 15(cid:3)
1(cid:3) Introduction ....................................................................................................................... 17(cid:3)
1.1(cid:3)Relevance ...................................................................................................................... 17(cid:3)
1.2(cid:3)Antibiotics in the environment: transport routes .......................................................... 18(cid:3)
1.2.1(cid:3)Antibiotics used in human medicine ................................................................... 19(cid:3)
1.2.2(cid:3)Antibiotics used in agriculture ............................................................................ 19(cid:3)
1.2.3(cid:3)Antibiotics used in aquaculture .......................................................................... 20(cid:3)
1.2.4(cid:3)Focus ................................................................................................................... 20(cid:3)
1.3(cid:3)Veterinary antibiotic behaviour .................................................................................... 21(cid:3)
1.4(cid:3)Objective ....................................................................................................................... 21(cid:3)
1.5(cid:3)Study Area .................................................................................................................... 21(cid:3)
1.6(cid:3)Approach ....................................................................................................................... 22(cid:3)
1.7(cid:3)Thesis outline ................................................................................................................ 23(cid:3)
2(cid:3) The overland journey of veterinary antibiotics: a review ............................................. 27(cid:3)
2.1(cid:3)Abstract ......................................................................................................................... 27(cid:3)
2.2(cid:3)Introduction ................................................................................................................... 28(cid:3)
2.3(cid:3)Focus and objective....................................................................................................... 28(cid:3)
2.4(cid:3)VAs of interest .............................................................................................................. 29(cid:3)
2.5(cid:3)VA behaviour ................................................................................................................ 31(cid:3)
2.5.1(cid:3)Sorption ............................................................................................................... 31(cid:3)
2.5.2(cid:3)Degradation ........................................................................................................ 34(cid:3)
2.6(cid:3)Environmental occurrence of VAs ................................................................................ 36(cid:3)
2.6.1(cid:3)Fertilizers ............................................................................................................ 37(cid:3)
2.6.2(cid:3)Soils ..................................................................................................................... 37(cid:3)
2.6.3(cid:3)Surface water systems ......................................................................................... 41(cid:3)
2.7(cid:3)Overland transport mechanisms .................................................................................... 43(cid:3)
2.7.1(cid:3)Surface runoff mechanisms ................................................................................. 44(cid:3)
2.7.2(cid:3)Soil erosion mechanisms ..................................................................................... 44(cid:3)
2.7.3(cid:3)Resistance to soil erosion.................................................................................... 45(cid:3)
2.7.4(cid:3)Predicting soil erosion ........................................................................................ 46(cid:3)
2.7.5(cid:3)Overland transport of VAs .................................................................................. 47(cid:3)
2.8(cid:3)VA contamination following overland transport .......................................................... 48(cid:3)
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2.9(cid:3)Concluding remarks ...................................................................................................... 49(cid:3)
3(cid:3) From agricultural fields to surface water systems: the overland transport of
veterinary antibiotics......................................................................................................... 53(cid:3)
3.1(cid:3)Abstract ......................................................................................................................... 53(cid:3)
3.2(cid:3)Introduction ................................................................................................................... 53(cid:3)
3.3(cid:3)Method and materials .................................................................................................... 55(cid:3)
3.4(cid:3)Results ........................................................................................................................... 56(cid:3)
3.5(cid:3)Discussion ..................................................................................................................... 57(cid:3)
4(cid:3) The veterinary antibiotic journey: comparing the behaviour of sulfadiazine,
sulfamethazine, sulfamethoxazole and tetracycline in cow excrement and two soils .. 59(cid:3)
4.1(cid:3)Abstract ......................................................................................................................... 59(cid:3)
4.2(cid:3)Introduction ................................................................................................................... 60(cid:3)
4.2.1(cid:3)Background ......................................................................................................... 60(cid:3)
4.2.2(cid:3)Current understanding of VA behaviour............................................................. 60(cid:3)
4.2.3(cid:3)Proposed conceptualisation of VA behaviour ..................................................... 61(cid:3)
4.2.4(cid:3)Approach ............................................................................................................. 62(cid:3)
4.3(cid:3)Method and Materials ................................................................................................... 64(cid:3)
4.3.1(cid:3)Cow excrement experiment ................................................................................. 64(cid:3)
4.3.2(cid:3)Soil experiment .................................................................................................... 64(cid:3)
4.3.3(cid:3)Preparation of soil liquid phase samples............................................................ 65(cid:3)
4.3.4(cid:3)Preparation of soil solid phase samples ............................................................. 66(cid:3)
4.3.5(cid:3)Methods of result interpretation ......................................................................... 66(cid:3)
4.4(cid:3)Results ........................................................................................................................... 68(cid:3)
4.4.1(cid:3)Cow excrement results ........................................................................................ 68(cid:3)
4.4.2(cid:3)Soil results ........................................................................................................... 71(cid:3)
4.4.3(cid:3)Speculated soil results......................................................................................... 71(cid:3)
4.5(cid:3)Discussion ..................................................................................................................... 72(cid:3)
4.5.1(cid:3)Cow excrement experiment ................................................................................. 72(cid:3)
4.5.2(cid:3)Soil experiment .................................................................................................... 76(cid:3)
4.5.3(cid:3)Realised conceptualisation of VA behaviour ...................................................... 77(cid:3)
4.6(cid:3)Conclusions ................................................................................................................... 78(cid:3)
5(cid:3) Numerically predicting the fate of veterinary antibiotics that are applied to
agricultural fields .............................................................................................................. 79(cid:3)
5.1(cid:3)Abstract ......................................................................................................................... 79(cid:3)
5.2(cid:3)Introduction ................................................................................................................... 80(cid:3)
5.3(cid:3)Method .......................................................................................................................... 81(cid:3)
5.3.1(cid:3)Concept of spatial and temporal discretization .................................................. 81(cid:3)
5.3.2(cid:3)Events .................................................................................................................. 82(cid:3)
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5.3.3(cid:3)VA behaviour ...................................................................................................... 82(cid:3)
5.3.4(cid:3)Mass budget ........................................................................................................ 83(cid:3)
5.3.5(cid:3)Depth concepts .................................................................................................... 84(cid:3)
5.3.6(cid:3)Time step initialisation ........................................................................................ 85(cid:3)
5.3.7(cid:3)Implementation of events and VA behaviour ...................................................... 85(cid:3)
5.3.8(cid:3)Concentrations .................................................................................................... 94(cid:3)
5.3.9(cid:3)Choice of surface runoff-soil erosion model ....................................................... 94(cid:3)
5.4(cid:3)Case study ..................................................................................................................... 95(cid:3)
5.4.1(cid:3)PESERA .............................................................................................................. 95(cid:3)
5.4.2(cid:3)VANTOM input data ........................................................................................... 97(cid:3)
5.4.3(cid:3)VANTOM results and discussion ........................................................................ 98(cid:3)
5.4.4(cid:3)Analysis ............................................................................................................. 105(cid:3)
5.5(cid:3)Concluding remarks .................................................................................................... 105(cid:3)
6(cid:3) The influence of fertilizer management on the transport of veterinary antibiotics by
surface runoff and eroded soil ........................................................................................ 109(cid:3)
6.1(cid:3)Abstract ....................................................................................................................... 109(cid:3)
6.2(cid:3)Introduction ................................................................................................................. 110(cid:3)
6.3(cid:3)Study Area .................................................................................................................. 111(cid:3)
6.3.1(cid:3)Geographical information ................................................................................ 111(cid:3)
6.3.2(cid:3)Fertilizer Usage ................................................................................................ 112(cid:3)
6.3.3(cid:3)Fertilizer restrictions ........................................................................................ 112(cid:3)
6.3.4(cid:3)VAs in fertilizer ................................................................................................. 113(cid:3)
6.3.5(cid:3)Spatial and temporal distribution of VAs.......................................................... 113(cid:3)
6.4(cid:3)Fertilizer sampling ...................................................................................................... 114(cid:3)
6.4.1(cid:3)Introduction....................................................................................................... 114(cid:3)
6.4.2(cid:3)Method .............................................................................................................. 115(cid:3)
6.4.3(cid:3)Results ............................................................................................................... 115(cid:3)
6.4.4(cid:3)Interpretation .................................................................................................... 116(cid:3)
6.4.5(cid:3)Conclusion: temporal trends ............................................................................ 117(cid:3)
6.5(cid:3)Numerical Modelling .................................................................................................. 122(cid:3)
6.5.1(cid:3)Introduction....................................................................................................... 122(cid:3)
6.5.2(cid:3)Scenario definition ............................................................................................ 122(cid:3)
6.5.3(cid:3)Input data .......................................................................................................... 124(cid:3)
6.5.4(cid:3)Results and discussion ...................................................................................... 126(cid:3)
6.5.5(cid:3)Analysis ............................................................................................................. 140(cid:3)
6.6(cid:3)Concluding remarks .................................................................................................... 142(cid:3)
7(cid:3) The overland transport of veterinary antibiotics: a synthesis .................................... 143(cid:3)
7.1(cid:3)Introduction ................................................................................................................. 143(cid:3)
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7.2(cid:3)Summary and synthesis of presented work ................................................................. 144(cid:3)
7.2.1(cid:3)Structure ............................................................................................................ 144(cid:3)
7.2.2(cid:3)Literature review (Chapter 2) ........................................................................... 145(cid:3)
7.2.3(cid:3)Water and sediment sampling (Chapter 3) ....................................................... 145(cid:3)
7.2.4(cid:3)Laboratory experiments (Chapter 4) ................................................................ 146(cid:3)
7.2.5(cid:3)Numerical model theory (Chapter 5) ................................................................ 146(cid:3)
7.2.6(cid:3)Numerical model application (Chapter 6) ........................................................ 147(cid:3)
7.3(cid:3)Research achievements ............................................................................................... 148(cid:3)
7.4(cid:3)Research limitations .................................................................................................... 150(cid:3)
7.5(cid:3)Recommendations and closing remarks...................................................................... 151(cid:3)
References .................................................................................................................................. 153(cid:3)
About the Author ...................................................................................................................... 161(cid:3)

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Abbreviations
Abbreviation Meaning
BD biogas digestate
d.s.c. dry solid content
SPE solid phase extraction
VA(s) veterinary antibiotic(s)

SAs Sulfonamides & Trimethoprim
SCP sulfachoropyridazine
SDM sulfadimethoxine
SDZ sulfadiazine
SGD sulfaguanidine
SMR sulfamerazine
SMZ sulfamethazine (as known as sulfadimidine)
SMX sulfamethoxazole
SMP sulfamethoxypyridazine
SPY sulfapyridine
STZ sulfathiazole
TPM trimethoprim

TCs Tetracyclines
CTC chlortetracycline
DTC doxycycline
OTC oxytetracycline
TC tetracycline

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