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Predicting Fuel Properties from Infrared Spectra THESIS ON CHEMISTRY AND CHEMICAL ENGINEERING G49 Predicting Fuel Properties from Infrared Spectra ZACHARIAH STEVEN BAIRD TALLINN UNIVERSITY OF TECHNOLOGY School of Engineering Department of Energy Technology This dissertation was accepted for the defense of the degree of Doctor of Philosophy in Chemical and Materials Technology on July 31th, 2017. Supervisor: Prof. Vahur Oja Department of Energy Technology, TTÜ Opponents: Prof. Dr. Selhan Karagoz Karabuk University, Turkey Dr. Mati Karelson Tartu University, Estonia Defense of the thesis: September 15, 2017 Declaration: Hereby I declare that this doctoral thesis, my original investigation and achievement, submitted for a doctoral degree at Tallinn University of Technology, has not been submitted for any other academic degree. ISSN 1406-4774 ISBN 978-9949-83-145-6 (publication) ISBN 978-9949-83-146-3 (PDF) This work is licensed under the Creative Commons Attribution-ShareAlike 4.0 International License. To view a copy of this license, visit http://creativecommons.org/licenses/by-sa/4.0/. © Copyright: Zachariah Baird, 2017 KEEMIA JA KEEMIATEHNIKA G49 Kütuse omaduste hindamine infrapunaspektrilt ZACHARIAH STEVEN BAIRD TALLINNA TEHNIKAÜLIKOOL Inseneriteaduskond Energiatehnoloogia instituut Doktoritöö on lubatud kaitsmisele filosoofiadoktori kraadi taotlemiseks keemia- ja materjalitehnoloogia erialal 31. juulil 2017. Juhendaja: prof Vahur Oja Energiatehnoloogia instituut, TTÜ Oponendid: prof Selhan Karagoz Karabuk University, Türki Dr. Mati Karelson Tartu Ülikool, Eesti Doktortöö kaitsmise aeg: 15. september, 2017 Deklaratsioon: Deklareerin, et see doktoritöö, mis on minu iseseisva töö tulemus, on esitatud Tallinna Tehnikaülikooli doktorikraadi taotlemiseks ja selle alusel ei ole varem taotletud doktori- või sellega võrdsustatud teaduskraadi. ISSN 1406-4774 ISBN 978-9949-83-145-6 (publication) ISBN 978-9949-83-146-3 (PDF) © Autoriõigus: Zachariah Baird, 2017 TABLE OF CONTENTS LIST OF PUBLICATIONS ................................................................................... 8 LIST OF ABBREVIATIONS ............................................................................... 9 LIST OF FIGURES ............................................................................................. 10 LIST OF TABLES .............................................................................................. 13 INTRODUCTION ............................................................................................... 14 1. FUEL PROPERTY PREDICTION – A REVIEW ........................................ 16 The need for property prediction .................................................................... 16 Approaches to fuel property prediction........................................................... 16 Collecting input data ................................................................................... 16 Data abstraction .......................................................................................... 17 Modeling the relationship ........................................................................... 18 Shale oil .......................................................................................................... 18 Property prediction for shale oil ...................................................................... 19 2. CHEMOMETRICS FOR FUEL PROPERTY PREDICTION ...................... 20 Overview of developments ............................................................................. 20 Properties predicted......................................................................................... 21 Fuel types used ................................................................................................ 21 Analytical method used for measuring input data ........................................... 22 Accuracy of the models ................................................................................... 22 Regression methods used ................................................................................ 24 3. THEORY ........................................................................................................ 25 The basis for predicting properties from chemical information ...................... 25 Overview of multivariate regression methods ................................................ 26 Partial least squares regression ....................................................................... 27 Support vector regression ................................................................................ 28 4. INFRARED MEASUREMENT SYSTEMS ................................................. 31 Mid or near infrared ........................................................................................ 31 Types of accessories........................................................................................ 31 Implementation in industrial processes ........................................................... 33 Wavelength separation methods ..................................................................... 33 5. CREATION OF PROPERTY DATABASE .................................................. 35 Samples used ................................................................................................... 35 Sample preparation ......................................................................................... 35 Distillation .................................................................................................. 35 Extraction .................................................................................................... 36 Measurement methods used ............................................................................ 36 Density ........................................................................................................ 37 Refractive index .......................................................................................... 38 Average boiling point ................................................................................. 38 Molecular weight ........................................................................................ 39 Hydrogen content ....................................................................................... 39 Carbon content ............................................................................................ 39 Sulfur content ............................................................................................. 40 Hydroxyl content ........................................................................................ 40 Pour point ................................................................................................... 40 Viscosity ..................................................................................................... 41 Infrared measurement procedure .................................................................... 41 6. INFRARED SPECTRA ................................................................................. 44 7. MODEL CREATION PROCESS .................................................................. 52 Error estimation .............................................................................................. 52 Outlier removal ............................................................................................... 53 Sample selection ............................................................................................. 54 Variable selection ............................................................................................ 60 Regression method .......................................................................................... 62 Model parameter optimization ........................................................................ 64 8. MODELS FOR TEMPERATURE INDEPENDENT PROPERTIES ........... 66 Structure parameters ....................................................................................... 66 Size parameters ............................................................................................... 69 Chemical composition ..................................................................................... 71 Other properties .............................................................................................. 76 6 9. MODELS FOR TEMPERATURE DEPENDENT PROPERTIES ................ 80 General approach ............................................................................................ 80 Density ............................................................................................................ 80 Viscosity ......................................................................................................... 81 10. PERFORMANCE OF THE MODELS .......................................................... 86 Accuracies of the models ................................................................................ 86 Causes underlying performance ...................................................................... 87 Comparison with bulk property correlations ................................................... 94 Comparison by fraction ................................................................................... 97 11. ADDITIONAL ISSUES FOR WIDER APPLICATION ............................... 99 Transfer of a model for use on other instruments ........................................... 99 Better basis for extrapolation to fuels from other sources ............................ 102 12. CONCLUSIONS .........................................................................................
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