biodegradation of synthetic polymers in the aquatic environment

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  • BIODEGRADATION OF SYNTHETIC POLYMERS IN

    THE AQUATIC ENVIRONMENT

    Dissertation zur Erlangung des akademischen Grades eines Doktors der

    Naturwissenschaften - Dr. rer. nat. - am Fachbereich II (Biologie/Chemie) der

    Universitt Bremen

    Vorgelegt von Jan P. Eubeler

    Bremen im April 2010

  • BIODEGRADATION OF SYNTHETIC POLYMERS IN THE AQUATIC ENVIRONMENT

    II|XVIII

    1. Gutachter Hr. Prof. Dr. Rudolf Amann (Universitt Bremen)

    2. Gutachter Fr. Dr. Sabine Zok (BASF SE Ludwigshafen)

    1. Prfer Hr. Prof. Dr. Michael W. Friedrich (Universitt Bremen)

    2. Prfer Hr. Prof. Dr. Thomas P. Knepper (Hochschule Fresenius, Idstein)

    Termin des ffentlichen Kolloquiums:

    21. Juni 2010, 13:30 Uhr, Alter Hrsaal, MPI fr Marine Mikrobiologie, Celsiusstr. 1, Bremen

    Eidesstattliche Erklrung

    gem. 6 (5) Nr. 1-3 Promotions-Ordnung der Universitt Bremen vom 14 Mrz 2007

    Hiermit erklre ich, das ich

    die Arbeit ohne unerlaubte fremde Hilfe angefertigt habe,

    keine anderen als die von mir angegebenen Quellen und Hilfsmittel benutzt habe und

    die den benutzten Werken wrtlich oder inhaltlich entnommenen Stellen als solche kenntlich gemacht

    habe.

    Grokarlbach, den 01. April 2010

    Jan P. Eubeler

  • BIODEGRADATION OF SYNTHETIC POLYMERS IN THE AQUATIC ENVIRONMENT

    III|XVIII

    "Bildung ist das, was brig bleibt, wenn man alles vergessen hat, was man

    gelernt hat. ()"

    (Werner Heisenberg)

    und was man dann wiederum zu erlernen bereit ist.

  • BIODEGRADATION OF SYNTHETIC POLYMERS IN THE AQUATIC ENVIRONMENT

    IV|XVIII

  • BIODEGRADATION OF SYNTHETIC POLYMERS IN THE AQUATIC ENVIRONMENT

    V|XVIII

    Acknowledgements

    First of all, I would like to thank both my supervisor Dr. Sabine Zok (BASF SE) and Prof. Dr. Thomas P. Knepper

    (Fresenius University of Applied Sciences) and my colleague and friend Dipl.-Ing. M. Bernhard for their help and

    cooperation on this project and all related topics.

    Furthermore I would like Prof. Dr. Allan D. Cembella (AWI Bremerhaven) for taking me as his doctoral student

    and being my supervisor. I wish him all the best for recovering from his very unfortunate accident.

    I also like to express my deepest gratitude to Prof. Dr. Rudolf Amann for taking over the position of Prof.

    Cembella and supporting me through final phase of my dissertation. Thanks also to Prof. Dr. Michael W.

    Friedrich for his expertise on my thesis. My gratitude goes also to Sara Kleindienst and Juliane Wippler for

    being part of the committee.

    I would like to express my gratitude especially to Helmut Schwarz, Stephan Hammer, Juergen Bachner, Karl-

    Heinz Ullrich, Arnold Lumpi Gottwald, Helene Froehlich and Andy Haupt (GV/TC), for their support and help

    every day in the Lab. Special thanks for the great time with you guys and the perfect Friday morning

    breakfast. I will always remember that!

    I am also most grateful to Dr. Christian Schtt and Hilke Dpke (BAH/AWI Helgoland/Bremerhaven) for the

    cooperation, their intensive and unlimited help and the good weeks I spent at AWI BAH.

    Special thanks go to Mrs. Frauke Ernst from University of Bremen. Thank you for your fast and constant support

    in every administrative aspect.

    I would like to thank BASF SE, especially GV/T as well as Mrs. Dr. Katrin Schwarz and her Team (E-EMV/Q) for

    funding my project and for their support. It was a pleasure to work with you.

    I also want to thank a lot of BASF staff for various help in my project:

    Jens Kampioni for sending me all Pluriol E type and Pluriol E care samples, MSc Motonori Yamamoto for

    supplying ECOFLEX, ECOVIO, MaterBi and PLA samples in various different versions. Thanks go as well to Dr.

    Joachim Fischer, Dr. Inge Langbein, Dr. Klaus Taeger and Dr. Peter Reuschenbach for inspiring talks and ideas.

    Thanks to Dr. Uwe Witt for supplying me with Oxo-PE samples and for discussions and literature and to Gert

    Asselman from BTC Specialty Chemical Distribution N.V./S.A. Belgium for sending me samples of PEG &

    MAPEG. Special thanks to Uwe Ruffer and Dr. Andrea Hrster from the Bioanalytical Department at BASF SE for

    analyzing my marine samples. I also want to thank Prof. Dr. Andreas Knkel and his team for their input on my

    review papers.

    I want to express special gratitude also in the name of BASF to Mr. Wittner and his team at Luisenpark

    Mannheim for their support and interest and for allowing myself to collect many, many seawater samples &

  • BIODEGRADATION OF SYNTHETIC POLYMERS IN THE AQUATIC ENVIRONMENT

    VI|XVIII

    microorganisms from their aquarium! Also, I would like to thank those involved in sending seawater samples

    from the North Sea near BASF Guesthouse at Sylt, Westerland to our laboratory for use in marine tests.

    Thanks to Dipl.-Phil., Dipl.-Soz.-Pd. Sylvia Bttger from HS Fresenius, Idstein for her big support in my search

    for literature. She has been always kind and never tired of sending me publications I could not get off the

    Internet.

    Thank you very much GDCh, SETAC, ASMS, DECHEMA e.V., ACS and all the other scientific societies. You were

    all being very cooperative and supportive through all my time as an undergrad and grad student! This is

    gratefully acknowledged and appreciated! Special Thanks to VCI/FCI for providing me with a scholarship for the

    SETAG/GDCh PGS-Course in Ecotoxicology. The course is done very well and I would like to thank all involved

    colleagues for their commitment.

    All the people I have forgotten to mention here may please forgive me. You have also participated in this work

    and you may remind me of that whenever you wish!

    Last but not least I want to thank my mom and dad and also my grandparents for always listening and being

    helpful and supportive. I am very grateful for many, many years of constant and unlimited support.

    I would also like to thank Hendrik Jacob, Manuela Peschka, Matthias Mcki Mckl and Stefan Kappner, as

    well as Holger Rinker, Frank Hess and Jrgen Diehl for the great hours we spent together (not only in the

    Promised Land) having lots of fun! And thanks to the BOSS and all his colleagues and friends that have

    delivered many days of beautiful reward being my winding wheel.

  • BIODEGRADATION OF SYNTHETIC POLYMERS IN THE AQUATIC ENVIRONMENT

    VII|XVIII

    Abstract

    Biodegradation of synthetic polymers can be a sophisticated property for intelligent and sustainable products

    that offer complex benefits for specific applications. There are many entry paths for synthetic polymers that

    can accumulate in the aqueous and especially marine environment and little is known about their

    biodegradation especially in the aquatic environment. The difficulties with determining biodegradation in those

    environments are based on the absence of appropriate methods and also the fact that these environments

    often prove low biodegradation rates. It is also complicated to detect biodegradation on polymeric substances

    because of the high molecular weight, water insolubility and difficult molecular structure making it hard to

    detect biodegradation products.

    This work provides an overview of the actual status of research regarding biodegradation, results and methods

    describing biodegradation of biodegradable polymers. The main focus of this study is to find out if standard

    biodegradation tests may be used for the evaluation of polymer biodegradation. Its aim is to identify difficulties

    and problems with these tests and to compare the biodegradation potential and biodegradation pathways in

    the marine and freshwater environment for a selection of polymer types.

    It is also investigated whether molecular or structural properties of the polymers influence the biodegradation

    in different environments and the possible pathways of biodegradation. Similarities and differences are

    identified and on a selection of the biodegradation tests an investigation of the microorganism community is

    performed to evaluate the use of molecular methods to discover influences of microorganisms on the

    biodegradation of polymers.

    Investigating available methods on how evaluation of biodegradation can be performed best in this special field

    is a first step in a new direction. It may be important for further development of representative test

    procedures. First facts on how biodegradation can be determined under the special circumstances are

    established based on standardized methods which are adapted to the requirements

    Three different types of carefully selected polymers and their degradation behaviour are evaluated based on

    OECD test guidelines. Compounds were selected based water solubility/insolubility and biodegradation

    potential:

    Poly(vinyl pyrrolidone) is selected because it is known to be recalcitrant and is investigated to observe

    differences and similarities in different tests and media when no biodegradation can be observed

    (negative control).

    Poly(ethylene glycol), a water soluble biodegradable polymer is investigated in broad molecular

    weight distribution ranging from molecular weights of 200 to almost 60000 gmol -1. Data from

    different aquatic compartments are compared to establish differences systematically.

  • BIODEGRADATION OF SYNTHETIC POLYMERS IN THE AQUATIC ENVIRONMENT

    VIII|XVIII

    The water insoluble biode

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