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Thermochemical Conversion of Lignocellulosic Biomass Into Biofuels with Aspen Plus Simulation

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Thermochemical Conversion of Lignocellulosic Biomass Into Biofuels with Aspen Plus Simulation MASTER THESIS IN CHEMICAL ENGINEERING Thermochemical conversion of lignocellulosic biomass into biofuels with Aspen Plus simulation Author: Ângelo Dinis Simões Nunes Supervisors: António Alberto Torres Garcia Portugal Lino de Oliveira Santos A thesis submitted in fulfilment of the requirements for the degree of Master of Science in the Department of Chemical Engineering September, 2015 “The existing scientific concepts cover always only a very limited part of reality, and the other part that has not yet been understood is infinite." Werner Heisenberg Resumo Nos últimos anos, a escassez de recursos fósseis tornou-se uma realidade importante. Aliada aos efeitos ambientais negativos que advêm com a exploração destes recursos, são necessárias alternativas. Nos últimos anos, houve um foco, liderado em grande parte pela Europa em encontrar alternativas aos combustíveis fósseis que sejam verdadeiramente viáveis, especialmente no sector dos transportes. O mercado dos transportes está a crescer rapidamente, muito devido à China e outros países emergentes, o que significa que a procura ligada aos combustíveis para transportes só irá aumentar. De modo a satisfazer esta procura, alternativas ao petróleo são necessárias e os biocombustíveis surgem como um importante recurso. No entanto, ainda existem muitos problemas associados ao processamento das matérias-primas, nomeadamente a biomass, em combustíveis que possam ser usados. Há também o benefício da valorização dos recursos endógenos ao nível económico, social e ambiental. Esta tese pretende descrever a pirólise de cinco tipos de madeira, que podem ser encontradas dentro de Portugal continental. Dois esquemas reaccionais foram testados para todas as amostras e modificações foram feitas de forma a melhor coincidir com resultados experimentais, tal levou ao estudo de um cenário optimizado. Os esquemas retirados da literatura foram usados sem modificações em simulações em Aspen Plus, e apresentaram grandes desvios em relação aos resultados experimentais, com desvios de rendimentos de açúcares e água acima de 15% em erro absoluto. Com as modificações introduzidas, a maior parte dos componentes simulados apresentaram um erro inferior a 2%, com a excepção do char, água e gás, com desvios na ordem dos 3-4%. Tendo a unidade uma capacidade de processamento de 90 ton/dia de biomass, o calor necessário para a pirólise está entre 1.6-1.8MW dependendo do tipo de biomassa, e para todos os casos há excesso de calor (entre 1.75-3MW). Uma análise de sensibilidade permitiu inferir que os esquemas reaccionais usados estão limitados tanto em termos de temperatura como tempo de residência. v Abstract In recent years, the scarcity of fossil fuels became an important reality. Allied with the negative environment consequences that come with exploration of these resources, alternatives are needed. In the last years, there has been a focus, driven mostly by Europe into finding truly viable alternatives to fossil fuels, specially in the transportation sector. Rapidly growing transportation markets in China and other developing countries means the demand for transportation fuel will only increase. In order to provide for the ever growing demand the alternative for oil is needed and the importance of biofuels is unquestionable. However there are many problems associated with processing of the feed materials, namely biomass, into usable fuels. Also, there are benefits in the valorization of endogenous resources, at the economical, social and environmental level. The present thesis aims at properly describing pyrolysis of five selected wood samples, that can typically be found within Portugal’s continental borders. Two reaction schemes will be tested for all the samples, and some modifications to better match experimental data, leading to an optimized scenario will also be studied. The schemes retrieved from the literature, used as is in an Aspen Plus simulation environment, present high deviation to experimental data, with water and sugar deviations above 15% in absolute error. When the modification are introduced, most of the components present an absolute error below 2%, with the exception of char, water and gas, which still show deviations in the 3-4% range. With a biomass processing capacity of 90 tons/day, the pyrolysis duty is around 1.6-1.8MW depending on the feedstock, and in all cases there is a heat surplus (between 1.75-3MW). Sensibility analysis shows that the used reaction schemes are limited both in temperature that can be used and residence time. vi Acknowledgements I would like to thank my supervisor, Dr. António Portugal for firstly captivating my interest in the subject, throughout the Energy and Biofuels classes lectured and thereafter, and secondly, in allowing me to purse this topic as my thesis, which allies two of my favourite subjects in chemical engineering: energy and numerical simulation. I would like to thank my other supervisor, Dr. Lino Santos, for his promptness in solving any student’s simulation problems, even if not at all related to the subject he teaches, and also for providing me with the LATEXtemplate to put this thesis together. To Mr. Rui Moreira for his help and tremendous expertise in anything Aspen Plus related, as well as lectures regarding thermochemical processes, where I could get a more deep insight of pyrolysis as well as gasification. I want to thank the Department of Chemical Engineering for all these five years where I’ve felt home and to everyone that I’ve come across and helped me along the way, being it my fellow students, professors or employees. I would like to acknowledge all my friends, to the ones I’ve met in Coimbra for sharing this wonderful experience that is the university life with me, and also helping me with my studies; the ones from Ansião, by always being there since I can remember, I’m sure there are no true friendship like yours anywhere else. And last but not least, to my family: my parents for the motivation given, support and strength to carry on, specially in the hardest moments, and to my brother, for his support throughout my academic life and promotion in the virtues of being a chemical engineer. Without you I couldn’t have done this. vii Contents Resumo v Abstract vi Acknowledgements vii List of Figures xi List of Tables xiii 1 Introduction 1 1.1 The transportation sector fuel problem . .2 1.2 Environmental aspects . .4 1.3 Synthetic fuels history and developments . .6 1.4 Biomass potential . .9 1.5 Motivation and objectives . 12 1.6 Thesis structure . 14 Bibliography . 15 2 State of the art 17 2.1 The fluidization principle . 17 2.1.1 Advantages and disadvantages of fluidized beds . 18 2.2 Gasification . 19 2.3 Pyrolysis . 22 2.3.1 Fast pyrolysis . 22 2.3.2 Bio-oil upgrading . 28 Bibliography . 32 3 Simulation 35 3.1 Kinetic parameters determination . 35 3.2 Reaction mechanism developments . 41 3.3 Selected reaction schemes . 44 3.4 Aspen Plus considerations . 51 3.4.1 Properties . 51 3.4.2 Simulation . 55 Bibliography . 61 ix x CONTENTS 4 Results and Discussion 67 4.1 Exploratory analysis . 68 4.2 Reaction parameters optimization . 80 4.3 Sensibility analysis . 86 Bibliography . 91 5 Conclusion and future work 93 Appendices 95 A Component yields 97 B Mass balances 121 List of Figures 1.1 World energy consumption for transportation sector projections up to 2040 by fuel type used [5]. .2 1.2 Energy Return On Investment (EROIs) for several energy sources [6]. .3 1.3 Global CO2 atmospheric concentration and fossil fuel emissions accounted per source [8][9]. .4 1.4 Air emissions relative to the EU28 zone and comparison with global CO2 emissions (top and right axis are respective to the global CO2 line) [10]. .5 1.5 Main conversion routes for fossil synthetic fuels. .6 2.1 Fluidized bed reactor concept. 18 2.2 Main types of gasification reactors. 20 2.3 Bubbling fluidized bed reactor. 24 2.4 Circulating fluidized bed reactor. 25 2.5 Principle of the rotating cone reactor (adapted from [21]). 26 2.6 Aston University Mark 2 ablative fast pyrolysis reactor (adapted from [5]). 27 2.7 Screw/augor fast pyrolysis reactor concept. 28 3.1 Broido’s multi-step cellulose pyrolysis scheme (1971) [45]. 42 3.2 Broido and Nelson cellulose pyrolysis scheme (1975) [46]. 42 3.3 Broido-Shafizadeh (B-S) cellulose pyrolysis scheme (1979) [48]. 42 3.4 Thurner-Mann biomass pyrolysis scheme (1981) [31]. 43 3.5 Koufopanos biomass pyrolysis scheme (1991) [51]. 43 3.6 Miller-Bellan biomass pyrolysis scheme (1997) [40]. 43 3.7 General reaction scheme for cellulose, as presented by Ranzi et al. [52]. 44 3.8 General reaction scheme for hemicellulose, as presented by Ranzi et al. [52]. 46 3.9 General reaction scheme for lignins, as presented by Ranzi et al. [52]. 46 3.10 Process flow diagram as seen in Aspen Plus. 52 4.1 Absolute error for the five biomass samples (S1 simulation). 69 4.2 Absolute error for the five biomass samples (S2 simulation). 71 4.3 Absolute error for the five biomass samples, reaction 2 with n = 0:5 (S1* simulation). 72 4.4 Absolute error for the five biomass samples, x = 0:3 (S3 simulation). 73 4.5 Absolute error for the five biomass samples, x = 0:3 (S4 simulation). 74 4.6 Absolute error as a function of x parameter for Pinus insignis (S5). 76 4.7 Absolute error in log scale for the different component classes and optimization scenarios (S5*). 77 4.8 Product yield for the 5 CSTR in series as a function of temperature (S6*, Bio4). 78 xi xii LIST OF FIGURES 4.9 Pyrolysis products yields as a function of reactor PYR-KIN residence time (Opt3 scenario from S5*). 79 4.10 Absolute error for the five biomass types used in the simulation (SX).
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