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Dissertation Ist in Der Hauptbibliothek Der Technischen Universität Wien Aufgestellt Und Zugänglich Die approbierte Originalversion dieser Dissertation ist in der Hauptbibliothek der Technischen Universität Wien aufgestellt und zugänglich. http://www.ub.tuwien.ac.at The approved original version of this thesis is available at the main library of the Vienna University of Technology. http://www.ub.tuwien.ac.at/eng DISSERTATION Liquid Fuel Production from Biomass Gasification Product Gas of the Biomass Gasifier at Güssing/Austria – Catalyst Characterisation, Desing, Construction and Operation of a Fischer Tropsch Pilot Plant ausgeführt zum Zwecke der Erlangung des akademischen Grades eines Doktors der technischen Wissenschaften unter der Leitung von Univ. Prof. Dipl.-Ing. Dr. techn. Hermann Hofbauer am Institut für Verfahrenstechnik, Umwelttechnik und Techn. Biowissenschaften (E 166) eingereicht an der Technischen Universität Wien Fakultät für Maschinenwesen und Betriebswissenschaften von Dipl.-Ing. Karl Ripfel-Nitsche Matrikelnummer 9426408 Obere Hauptstrasse 15 2305 Eckartsau Wien, im April 2017 ................................. Karl Ripfel-Nitsche Vorwort und Danksagung ______________________________________________________________________ Vorwort und Danksagung Die vorliegende Arbeit ist im Zuge meiner Tätigkeit als Forschungsassistent am Institut für Verfahrenstechnik, Umwelttechnik und Technische Biowissenschaften der Technischen Universität Wien entstanden. In dieser Arbeit werden die bisherigen Entwicklungen für erneuerbare flüssige Kraftstoffe dargestellt. Mit Hilfe der durchgeführten Arbeiten soll ein möglicher neuer Weg zur Erlangung von flüssigen Kraftstoffen aus Biomasse gezeigt werden. Der zweite Teil der Arbeit, welcher in den Jahren 2004-2007 entstand, zeigt die praktische Umsetzung dieses Vorhabens. Im dritten Teil werden die Erkenntnisse zusammengefasst und soll die möglichen Potentiale der Fischer Tropsch Synthese in Kombination mit einer Biomassedampfvergasung aufzeigen. Ich möchte allen danken, die am Entstehen dieser Arbeit mitgewirkt haben. Besonders danke ich: Hermann Hofbauer für die Aufnahme und Anstellung als Forschungsassistenten und der gegebenen Möglichkeit, meine Dissertation unter seiner Anleitung durchzuführen. Ich danke ihm für die zahlreichen fachlichen Diskussionen und die mir zugestandene Freiheit bei der Gestaltung der Arbeit. Herrn Reinhard Rauch möchte ich für die intensive Betreuung bei der Umsetzung der Arbeit am Institut in Wien sowie in Güssing und den vielen konstruktiven Diskussionen bedanken. Herrn Alain Kienneman und seinem Team auf der „Université de Strasbourg“ für die herzliche Aufnahme und Betreuung für den Zeitraum der Arbeiten zur Charakterisierung der Fischer Tropsch Katalysatoren in Frankreich. Herren Tobias Pröll für die vielen Anregungen und Hinweise im Hinblick auf das Verfassen der wissenschaftlichen Arbeit. Den Diplomanden Herren Niall O Brien und Markus Goritschnig die durch Ihren engagierten Einsatz am Entstehen dieser Arbeit mitgewirkt haben. Besonderen Dank gilt Herren Reinhard Koch und seinem Team des Biomassekraftwerkes in Güssing die durch Ihre Kooperation wesentlich am Entstehen dieser Arbeit teilhaben. Meinen Kollegen am Institut für die vielen geistreichen, unterhaltsamen und motivierenden Stunden während und nach der Arbeit. Danken möchte ich an dieser Stelle auch meinen Eltern die mir meine Ausbildung ermöglicht haben. Nicht zuletzt möchte ich mich bei meiner Frau Laura für die Korrektur in englischer Sprache und der moralischen Unterstützung während der Zeit des Verfassens der Arbeit bedanken. Kurzfassung Kurzfassung Ziel der Arbeit ist es, aus erneuerbarer Biomasse flüssige Kraftstoffe herzustellen. Um keine Konkurrenz zu konventionellen Agrarflächen darzustellen soll als Ausgangsstoff Holz dienen. Weiteres soll die Technologie in regionale Biomasse- kraftwerke integrierbar sein. Eine Fischer Tropsch Versuchsanlage wurde geplant, errichtet und betrieben in Güssing (Österreich). Es wurden Langzeitversuche mit dem Produktgas des Biomassedampfvergasers durchgeführt. Verschiedene Katalysatoren für die Fischer Tropsch Synthese wurden charakterisiert und getestet. Die hergestellten Fischer Tropsch Produkte wurden analysiert, unter anderem auf den Einsatz in Verbrennungs- kraftmotoren. Begleitend zu der Versuchsanlage in Güssing wurde ein Kaltmodell zum 3-Phasen-Strömungsreactor (Slurry-Reactor) errichtet. Eine Analysenmethode wurde entwickelt um die Katalysatorverteilung im Slurryreaktor zu beurteilen. Die Analysenergebnisse von den Fischer Tropsch Produkten, hergestellt von Kobalt basierenden Katalysatoren, ergeben einen qualitativ hochwertigen Kraftstoff. Die Eigenschaften des Kraftstoffes bei niedriger Temperatur müssen jedoch noch durch weitere Verfahrensschritte verändert werden um alle Anforderungen für Dieselkraft- stoffe zu erfüllen. Eine weitere entscheidende Erkenntnis ist der Bedeutung von einer Produktgasreinigung um den Katalysator vor Vergiftung zu schützen. Es wurde erkannt dass die Konzentration an Schwefelverbindungen im Synthesegas unter 10 ppbv zu liegen hat um dauerhaft die Synthese zu betreiben. Es konnte gezeigt werden, dass die Produktion von hoch qualitativen Kraftstoffen mit der Hilfe der Fischer Tropsch Synthese ausgehend von holzbasierender Biomasse möglich ist. Weiteres wurde erkannt, dass es der Kombination von verschiedenen Reinigungsschritten bedarf, um den Katalysator vor Inaktivierung bzw. Vergiftung zu schützen. Die Entfernung von Schwefelverbindungen wird nach wie vor eine entscheidende Rolle im Bereich der Fischer Tropsch Synthese mit Produktgas einer Biomassedampfvergasung spielen. Abstract __________________________________________________________________________ Abstract Aim of this work is to synthesise renewable liquid fuel of high quality. The basic material should be woody biomass so that no competition to agricultural space arises. Further, the technology should be integrated into local biomass power plant. A pilot plant for production of Fischer Tropsch fuel was designed, erected and continuously operated along the biomass stem gasification plant located at Güssing Austria. Different Fischer Tropsch catalysts have been characterised and tested in the pilot plant. The Fischer Tropsch products have been analysed, also with the focus on the applicability as automotive diesel fuel. Accompanying the pilot plant design phase, a cold model of the three phase slurry Fischer Tropsch reactor has been built. A method has been developed to measure catalyst distribution in the slurry phase. The results are showing that the obtained Fischer Tropsch fuel from cobalt catalysts is of high quality and fulfils nearly all demands of diesel fuel. Some refining steps would be necessary to fulfil all demands like the low temperature parameters of the fuel. However the Fischer Tropsch fuel from the iron based catalyst would need more refining steps to fulfil all parameters. A further learning from the operation of the pilot plant is that the gas cleaning of the synthesis gas upstream of the Fischer Tropsch reactor is of crucial importance. Above all the separation of sulphur compounds from the syngas is necessary. The concentration of sulphur compounds should be less then 10 ppbv in the Fischer Tropsch feed stream. It could be demonstrated that high quality fuel can be produced via Fischer Tropsch synthesis from the product gas of a biomass gasifier. The protection of the catalyst from poisoning is possible applying a combination of different gas cleaning steps. Sulphur removal will continue to be a challenge in Fischer Tropsch synthesis operated with product gas of a biomass gasification plant. Content __________________________________________________________________________________ Content 1 Introduction .................................................................................................... 5 1.1 Motivation .................................................................................................................... 5 1.2 Objectives ..................................................................................................................... 6 1.3 Formulation of the problem .......................................................................................... 6 1.4 Structure of the work .................................................................................................... 7 2 Literature review ............................................................................................ 7 2.1 Biofuels ........................................................................................................................ 7 2.1.1 Background ....................................................................................................................... 7 2.1.2 First generation ................................................................................................................. 9 2.1.3 Second generation .......................................................................................................... 10 2.2 Economic considerations ............................................................................................ 12 2.3 The history of Fischer Tropsch .................................................................................. 13 2.4 Previous Fischer Tropsch developments .................................................................... 13 2.5 2nd generation of biomass to liquid plants .................................................................. 14 2.5.1 CHOREN (Freiberg, Germany) .....................................................................................
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