Fate of the antibiotic sulfadiazine in Yangtze River sediments [Elektronische Ressource] : transformation, sorption and transport / Nan Meng

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• Publié par: rheinisch-westfalischen_technischen_hochschule_-rwth-_aachen
• Publié le: 01 janvier 2011
• Nombre de lectures: 43
• Langue: Deutsch
• Poids de l'ouvrage: 1 Mo

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Fate of the Antibiotic Sulfadiazine in Yangtze River
Sediments:
Transformation, Sorption and Transport


Von der Fakultät für Mathematik, Informatik und Naturwissenschaften der
RWTH Aachen University zur Erlangung des akademischen Grades
eines Doktors der Naturwissenschaften genehmigte Dissertation

vorgelegt von

Master der Naturwissenschaften


Nan Meng

Aus Dalian, China

Berichter: PD Dr. Erwin Klumpp
Prof. Dr. Andreas Schäffer

Tag der müdlichen Prüfung: 11. O ktober 2010

Diese Dissertation ist auf den Internetseiten der Hochschulbibliothek
online verfügbar.
Forschungszentrum Jülich GmbH
Institute of Bio- and Geosciences (IBG)
Agrosphere (IBG-3)
Fate of the Antibiotic Sulfadiazine in Yangtze
River Sediments: Transformation, Sorption and
Transport
Nan Meng
Schriften des Forschungszentrums Jülich
Reihe Energie & Umwelt / Energy & Environment Band / Volume 120
ISSN 1866-1793 ISBN 978-3-89336-736-8Bibliographic information published by the Deutsche Nationalbibliothek.
The Deutsche Nationalbibliothek lists this publication in the Deutsche
Nationalbibliografie; detailed bibliographic data are available in the
Internet at http://dnb.d-nb.de.
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Copyright: Forschungszentrum Jülich 2011
Schriften des Forschungszentrums Jülich
Reihe Energie & Umwelt / Energy & Environment Band / Volume 120
D 82 (Diss.,RWTH Aachen University, 2010)
ISSN 1866-1793
ISBN 978-3-89336-736-8
Neither this book nor any part of it may be reproduced or transmitted in any form or by any
means, electronic or mechanical, including photocopying, microfilming, and recording, or by any
information storage and retrieval system, without permission in writing from the publisher.Affirmation


Hereby I affirm that the presented doctoral thesis is my own work without any inadmissible
help by a third party and without using any other means than indicated. Thoughts that were
taken from other sources are indicated as such. This thesis has not been presented to any other
examination board in this or a similar form.




Jülich, 30 June 2010

Nan Meng







First referee: PD Dr. Erwin Klumpp

Second referee: Prof. Dr. Andreas Schäffer










ABSTRACT
Abstract
Sulfadiazine [4-amino-N-(2-pyrimidinyl) benzene sulfonamide] (SDZ) belongs to the widely
used antibiotic veterinary pharmaceuticals. After excretion by animals, these substances and
their transformation products are released into agricultural soils and adjacent environmental
compartments through the use of manure and sludge as fertilizer. Knowledge of the fate of
antibiotics in sediment and soil is crucial for assessing their environmental risk. Especially in
China, the behavior of antibiotics in river water and sediment is still poorly known. Therefore,
laboratory studies including batch and column experiments were performed to investigate the
transformation, sorption and transport behavior of SDZ in Yangtze sediments and their
components, such as minerals (goethite, illite, SiO , Al O ) and organic matter. 2 2 3

Three abiotic transformation products were only detected in the SDZ-goethite system under
the exclusion of light. All these products were found to be SO extrusion from SDZ. One of 2
these products was a new unknown transformation product, and the other two were identified
by mass spectrometry as 4-(2-iminopyrimidin-1(2H)-yl)aniline and p-(pyrimidin-2-
yl)aminoaniline. A ligand exchange mechanism was assumed for the surface interaction
between SDZ and goethite. A possible transformation pathway was proposed on the basis of
monodentate inner-sphere complexation and an intramolecular S reaction. N

Sorption kinetic data were fitted well by first order kinetics. Two days contact time was
chosen to avoid degradation of SDZ in sorption experiments. Nearly all the adsorption
isotherms determined in this study were nonlinear and could be best described by the
Freundlich adsorption isotherm. Surface area and pH were found to be the dominant factors
for SDZ sorption on minerals. Additionally, organic matter plays an important role in SDZ
sorption on sediments. Reversible sorption was observed for minerals (Al O and illite) and 2 3
desorption hysteresis occurred on most sediments. It was assumed that desorption was started
before adsorption had been completed (non-equilibrium conditions) and slow desorption of
SDZ from the sorbents. Sorption distribution coefficients (K ) for SDZ on sediments were low d
-1(ranging from 0.3 to 1.1 L kg ), which indicates that SDZ would be highly mobile in
sediments. The rate-limited sorption (RLS) model was successfully used to describe sorption
data in this study. The modeling results suggested that the adsorption and desorption rates are
the dominant factors for hysteresis of SDZ on sediments. In general, this experimental
IABSTRACT
procedure combined with the modeling presented here is recommended for adsorption
/desorption studies of unstable chemicals like antibiotics in terrestrial systems.

Transport of SDZ was investigated in sediment columns with varying flow rates and input
concentrations. Only weak retardation was found, which is in agreement with the low sorption
amounts and low K values in batch experiments. Column data were modeled successfully by d
the equilibrium convective dispersion equation (CDE). The retardation factor R obtained from
this model was about 50% lower than that calculated from the K values of batch experiments. d
One reason is the loss of active sorption sites due to the release of colloids such as dissolved
organic matter and minerals during conditioning of the sediment column. This is an important
finding with respect to a new recommendation for transport experiments with sediments.



























IITABLE OF CONTENTS
Table of contents

Abstract......................................................................................................................................I

List of Figures .........................................................................................................................VI

List of Tables...........................................................................................................................IX

Abbreviations........................................................................................................................... X

Symbols ...................................................................................................................................XI

Chapter 1
Introduction and objectives of this thesis...........................................................................- 1 -
1.1 Sulfonamides (antibiotic pharmaceuticals) in the terrestrial and aquatic environment.................... - 1 -
1.2 An important aquatic environment: Yangtze River and Three Gorges Reservoir............................. - 4 -
1.3 Research objectives and outline of this thesis .................................................................................. - 5 -

Chapter 2
Theoretical background.......................................................................................................- 7 -
2.1 Sulfadiazine as sorptive in aqueous solution.................................................................................... - 7 -
2.2 Surface properties of goethite........................................................................................................... - 8 -
2.3 Stability of sulfadiazine in the aquatic and terrestrial environment ............................................... - 10 -
2.4 Theory of sorption...........................................................................................................................- 11 -
2.4.1 Adsorption isotherm .................................................................................................................- 11 -
2.4.2 Sorption kinetics...................................................................................................................... - 14 -
2.4.3 Sorption of sulfonamides......................................................................................................... - 15 -
2.4.4 Desorption Hysteresis.............................................................................................................. - 19 -
2.5 Ad/desorption modeling ................................................................................................................. - 20 -
2.5.1 Rate-limited sorption (RLS)..........