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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

Effect of the addition of different waste carbonaceous materials on coal gasification in CO2 atmosphere

Parvez, A.M., Mujtaba, Iqbal M., Pang, C., Lester, E.H., Wu, T. 29 April 2016 (has links)
Yes / In order to evaluate the feasibility of using CO2 as a gasifying agent in the conversion of carbonaceous materials to syngas, gasification characteristics of coal, a suite of waste carbonaceous materials, and their blends were studied by using a thermogravimetric analyser (TGA). The results showed that CO2 gasification of polystyrene completed at 470 °C, which was lower than those of other carbonaceous materials. This behaviour was attributed to the high volatile content coupled with its unique thermal degradation properties. It was found that the initial decomposition temperature of blends decreased with the increasing amount of waste carbonaceous materials in the blends. In this study, results demonstrated that CO2 co-gasification process was enhanced as a direct consequence of interactions between coal and carbonaceous materials in the blends. The intensity and temperature of occurrence of these interactions were influenced by the chemical properties and composition of the carbonaceous materials in the blends. The strongest interactions were observed in coal/polystyrene blend at the devolatilisation stage as indicated by the highest value of Root Mean Square Interaction Index (RMSII), which was due to the highly reactive nature of polystyrene. On the other hand, coal/oat straw blend showed the highest interactions at char gasification stage. The catalytic effect of alkali metals and other minerals in oat straw, such as CaO, K2O, and Fe2O3, contributed to these strong interactions. The overall CO2 gasification of coal was enhanced via the addition of polystyrene and oat straw.
2

The influence of CO₂ on the steam gasification rate of a typical South African coal / Gillis J.D. Du Toit.

Du Toit, Gillis Johannes Dekorte January 2013 (has links)
It is recognised that the reactions with steam and CO2 are the rate limiting step during coal gasification, and a vast number of studies has been dedicated to the kinetics of these reactions. Most studies were carried out by using a single reactant (CO2 or H2O), either pure or diluted with an inert gas. Research using gas mixtures of CO2 and steam and their effects on gasification kinetics have been undertaken but are limited. The objective of this study is to determine the effects of CO2 on the steam gasification rate of a typical Highveld seam 4 coal. The South African medium ranked high volatile bituminous coal was charred at 950 °C. 2.0 g samples of ± 1 mm particles were analysed in a modified large particle thermo gravimetric analyser under various reactant gas concentrations. Experiments were conducted at atmospheric pressure (87.5 kPa) and temperatures from 775 to 900 °C, such that the conversion rate was controlled by chemical reaction. Reagent mixtures of steam-N2, steam-CO2 and CO2-N2 at concentrations of 25-75 mol%, 50-50 mol%, 75-25 mol% and 100 mol% were investigated. Arrhenius plots for steam and CO2 gasification produced activation energy values of 225 ± 23 kJ/mol and 243 ± 32 kJ/mol respectively. The calculated reaction orders with respect to reagent partial pressure were 0.44 ± 0.08 and 0.56 ± 0.07 for steam and CO2 respectively. Comparisons of the experimental data showed a higher reaction rate for the steam-CO2 mixtures compared to steam-N2 experiments. The semi empirical Wen model (m = 0.85) with an additive Langmuir-Hinshelwood styled rate equation predicted the mixed reagent gasification accurately. Reaction constants that were determined from the pure reactant experiments could directly be applied to predict the results for the experiments with mixtures of steam and CO2. The conclusion was made that under the investigated conditions steam and CO2 reacts simultaneously on different active sites on the char surface. / Thesis (MIng (Chemical Engineering))--North-West University, Potchefstroom Campus, 2013.
3

The influence of CO₂ on the steam gasification rate of a typical South African coal / Gillis J.D. Du Toit.

Du Toit, Gillis Johannes Dekorte January 2013 (has links)
It is recognised that the reactions with steam and CO2 are the rate limiting step during coal gasification, and a vast number of studies has been dedicated to the kinetics of these reactions. Most studies were carried out by using a single reactant (CO2 or H2O), either pure or diluted with an inert gas. Research using gas mixtures of CO2 and steam and their effects on gasification kinetics have been undertaken but are limited. The objective of this study is to determine the effects of CO2 on the steam gasification rate of a typical Highveld seam 4 coal. The South African medium ranked high volatile bituminous coal was charred at 950 °C. 2.0 g samples of ± 1 mm particles were analysed in a modified large particle thermo gravimetric analyser under various reactant gas concentrations. Experiments were conducted at atmospheric pressure (87.5 kPa) and temperatures from 775 to 900 °C, such that the conversion rate was controlled by chemical reaction. Reagent mixtures of steam-N2, steam-CO2 and CO2-N2 at concentrations of 25-75 mol%, 50-50 mol%, 75-25 mol% and 100 mol% were investigated. Arrhenius plots for steam and CO2 gasification produced activation energy values of 225 ± 23 kJ/mol and 243 ± 32 kJ/mol respectively. The calculated reaction orders with respect to reagent partial pressure were 0.44 ± 0.08 and 0.56 ± 0.07 for steam and CO2 respectively. Comparisons of the experimental data showed a higher reaction rate for the steam-CO2 mixtures compared to steam-N2 experiments. The semi empirical Wen model (m = 0.85) with an additive Langmuir-Hinshelwood styled rate equation predicted the mixed reagent gasification accurately. Reaction constants that were determined from the pure reactant experiments could directly be applied to predict the results for the experiments with mixtures of steam and CO2. The conclusion was made that under the investigated conditions steam and CO2 reacts simultaneously on different active sites on the char surface. / Thesis (MIng (Chemical Engineering))--North-West University, Potchefstroom Campus, 2013.
4

Gasification and combustion kinetics of typical South African coal chars / Mpho Rambuda

Rambuda, Mpho January 2015 (has links)
An investigation was undertaken to compare the kinetics of combustion and gasification reactions of chars prepared from two South African coals in different reaction atmospheres: air, steam, and carbon dioxide. The two original coals were characterised as vitrinite-rich (Greenside) and inertinite-rich (Inyanda) coals with relatively low ash content (12.5-16.7 wt. %, adb). Chars were prepared from the parent coals under nitrogen atmosphere at 900 °C. Characterisation results show that the volatiles and moisture were almost completely driven off from the parent coals, indicating that the pyrolysis process was efficient. Physicalstructural properties such as porosity and surface area generally increased from the parent coals to the subsequent chars. The heterogeneous char-gas reactions were conducted isothermally in a TGA on ~1 mm size particles. To ensure that the reactions are under chemical reaction kinetic control regime, different temperatures zones were selected for the three different reaction atmospheres. Combustion reactivity experiments were carried out with air in the temperature range of 387 °C to 425 °C; gasification reactivity with pure steam were conducted at higher temperatures (775 °C - 850 °C) and within 825 °C to 900 °C with carbon dioxide. Experimental results show differences in the specific reaction rate with carbon conversion in different reaction atmospheres and char types. Reaction rates in all three reaction atmospheres were strongly dependent on temperature, and follow the Arrhenius type kinetics. All the investigated reactions (combustion with air and gasification with CO2 and steam) were found to be under chemical reaction control regime (Regime I) for both chars. The inertinite-rich coals exhibit longer burn-out time than chars produced from vitrinite-rich coals, as higher specific reaction rate were observed for the vitrinite-rich coals in the three different reaction atmospheres. The determined random pore model (RPM) structural parameters did not show any significant difference during steam gasification of Greenside and Inyanda chars, whereas higher structural parameter values were observed for Greenside chars during air combustion and CO2 gasification (ψ > 2). However a negative ψ value was determined during CO2 gasification and air combustion of Inyanda chars. The RPM predictions was validated with the experimental data and exhibited adequate fitting to the specific rate of reaction versus carbon conversion plots of the char samples at the different reaction conditions chosen for this study. The activation energy determined was minimal for air and maximum for CO2 for both coals; and ranged from 127-175 kJ·mol-1 for combustion, 214-228 kJ·mol-1 and 210-240 kJ·mol-1 for steam and CO2 gasification respectively. / MIng (Chemical Engineering), North-West University, Potchefstroom Campus, 2015
5

Gasification and combustion kinetics of typical South African coal chars / Mpho Rambuda

Rambuda, Mpho January 2015 (has links)
An investigation was undertaken to compare the kinetics of combustion and gasification reactions of chars prepared from two South African coals in different reaction atmospheres: air, steam, and carbon dioxide. The two original coals were characterised as vitrinite-rich (Greenside) and inertinite-rich (Inyanda) coals with relatively low ash content (12.5-16.7 wt. %, adb). Chars were prepared from the parent coals under nitrogen atmosphere at 900 °C. Characterisation results show that the volatiles and moisture were almost completely driven off from the parent coals, indicating that the pyrolysis process was efficient. Physicalstructural properties such as porosity and surface area generally increased from the parent coals to the subsequent chars. The heterogeneous char-gas reactions were conducted isothermally in a TGA on ~1 mm size particles. To ensure that the reactions are under chemical reaction kinetic control regime, different temperatures zones were selected for the three different reaction atmospheres. Combustion reactivity experiments were carried out with air in the temperature range of 387 °C to 425 °C; gasification reactivity with pure steam were conducted at higher temperatures (775 °C - 850 °C) and within 825 °C to 900 °C with carbon dioxide. Experimental results show differences in the specific reaction rate with carbon conversion in different reaction atmospheres and char types. Reaction rates in all three reaction atmospheres were strongly dependent on temperature, and follow the Arrhenius type kinetics. All the investigated reactions (combustion with air and gasification with CO2 and steam) were found to be under chemical reaction control regime (Regime I) for both chars. The inertinite-rich coals exhibit longer burn-out time than chars produced from vitrinite-rich coals, as higher specific reaction rate were observed for the vitrinite-rich coals in the three different reaction atmospheres. The determined random pore model (RPM) structural parameters did not show any significant difference during steam gasification of Greenside and Inyanda chars, whereas higher structural parameter values were observed for Greenside chars during air combustion and CO2 gasification (ψ > 2). However a negative ψ value was determined during CO2 gasification and air combustion of Inyanda chars. The RPM predictions was validated with the experimental data and exhibited adequate fitting to the specific rate of reaction versus carbon conversion plots of the char samples at the different reaction conditions chosen for this study. The activation energy determined was minimal for air and maximum for CO2 for both coals; and ranged from 127-175 kJ·mol-1 for combustion, 214-228 kJ·mol-1 and 210-240 kJ·mol-1 for steam and CO2 gasification respectively. / MIng (Chemical Engineering), North-West University, Potchefstroom Campus, 2015
6

Influence of Potassium on Gasification Performance

Rasol, Hepa January 2016 (has links)
To release energy from chemically stored energy in the biomass was the new investigation in recent years. Utilizing of biomass for this purpose occur in two different ways, directly by burning (combustion) the biomass and indirectly by pyrolysis process which will convert the biomass to three main products, bio- tar, bio- char and synthetic gas. Biomass contains different amount of inorganic compound, especially alkali metals which causes some diverse impacts on combustion, pyrolysis and gasification process such as corrosion, agglomeration and fouling problems. This project aims to investigate the effect of K2CO3 on the pyrolysis and gasification processes of three different types of fuel; wood pellets, forest residue pellets and synthetic waste pellets at three different temperatures, 750 °C, 850 °C and 900 °C respectively. The purpose of this work to study and clarify the influence of K2CO3 on char yield, tar yield and tar compositions and the gasification rate and the reactivity of different fuels char. The pyrolysis process was carried out in a fluidized bed reactor during 2 minutes and the products were tar, char and synthetic gas. In this project interested in char and tar only. Char yield calculated and the results shows the char yield increase with increasing of [K2CO3]. While the tar analysis carried on GC- MS instrument at HB to study the tar yield and compositions. The results showed that potassium carbonate has not so much effect on tar yield and its composition. The last part was gasified the char in TGA with steam and CO2 as oxidizing media to study the influence of [K2CO3] on gasification rate and the reactivity of char samples at different temperatures. The result showed the [K2CO3] has inhibitory effect on gasification rate and the reactivity.
7

Efeito das principais variáveis do processo de fabricação sobre as propriedades de briquetes de misturas de carvão fóssil e carvão vegetal para uso siderúrgico. / Effect of the main process variables on the proprieties of briquettes of mixtures of coal and charcoal for steelmaking.

Varon Cardona, Lina Maria 28 September 2017 (has links)
A utilização de briquetes de misturas de carvão fóssil e biomassa em substituição ao coque como agente redutor pode contribuir para a diminuição das emissões de CO2 à atmosfera no processo de redução de minério de ferro. O fenômeno do amolecimento e fluidificação do carvão fóssil durante o aquecimento permite que o mesmo absorva certa quantidade de materiais inertes à coqueificação durante o tratamento térmico. O objetivo deste trabalho é correlacionar o efeito das principais variáveis de processo de fabricação (temperatura e tempo de tratamento térmico, tamanho de partícula dos componentes, porosidade e proporção de carvão vegetal e carvão fóssil) sobre as propriedades obtidas (resistência mecânica e reatividade ao CO2) de briquetes compostos de misturas de carvão fóssil e carvão vegetal, para uso na indústria siderúrgica. Briquetes de dois formatos diferentes foram preparados em matriz cilíndrica e em maquina briquetadeira e tratados termicamente em forno vertical aquecido com resistência elétrica sob atmosfera de nitrogênio. A resistência à compressão dos briquetes foi analisada em função das seguintes variáveis: proporção de carvão fóssil e carvão vegetal, taxa de aquecimento do tratamento térmico e tamanho de partícula dos carvões. A reatividade ao CO2 dos briquetes tratados termicamente foi analisada em função das seguintes variáveis: temperatura de ensaio e vazão de CO2. Foram comparados os resultados obtidos de ambos os formatos de briquetes. Com o aumento da proporção de carvão vegetal nos briquetes cilíndricos de biocoque, a densidade aparente e a resistência à compressão após tratamento térmico aumentaram para as misturas contendo 5, 10 e 15% de carvão vegetal. A partir dessa composição (15% de carvão vegetal) tanto a densidade final quanto a resistência à compressão apresentaram diminuição. Encontrou-se que tanto os briquetes cilíndricos a verde quanto os briquetes tratados termicamente apresentam perda de resistência mecânica com o aumento do tamanho de partícula do carvão fóssil. Os melhores valores de resistência à compressão foram obtidos em briquetes feitos com carvão fóssil em mistura de 15% em peso de carvão vegetal, tamanho de partícula abaixo de 0,044 mm, tratados termicamente a 1100°C durante 8 horas. Com o aumento na adição de carvão vegetal nos briquetes compostos de carvão fóssil e carvão vegetal, observou-se um aumento da reatividade do biocoque ao CO2. As micrografias dos briquetes tratados termicamente mostraram que a textura dos briquetes tende a ser mais homogênea com aumento de carvão vegetal de madeira na mistura. Os briquetes de biocoque fabricados em briquetadeira permitiram a ampliação do processo de fabricação de briquetes a uma escala laboratorial maior e mostraram a viabilidade industrial na fabricação do biocoque. Encontrou-se que a adição de carvão vegetal de madeira na mistura influencia diretamente na resistência a compressão e a reatividade ao CO2, devido a diferentes fatores como a composição das cinzas da madeira, a diminuição da fluidez devido à ação do inerte na mistura a carbonizar, a formação de uma estrutura porosa dentro da matriz carbonosa. Não encontrou-se correlação entre o índice de alcalinidade dos briquetes e sua reatividade ao CO2. / The substitution of metallurgical coke by briquetted mixtures of coal and biomass as a reducing agent can lower the emissions of greenhouse gases (CO2) in the iron and steelmaking industry. The thermal plasticity of the coking coal can be used to absorb an amount of inert materials during heat treatment. The objective of this study is to correlate the effect of the main processes variables (heat treatment temperature and duration, particle size of the materials, porosity and coal and charcoal ratio) on the properties (compressive strength and CO2 reactivity) of briquetted mixtures of coal and charcoal. Two types of briquettes were produced, one in a cylindrical die and another in a laboratory briquetting machine. The briquettes were heat treated in a vertical electrical furnace under nitrogen atmosphere. The compressive strength of the briquettes was analyzed as a function of the following variables: coal and charcoal ratio, heating rate and particle size. The CO2 reactivity of the heat treated briquettes was analyzed as a function of the following variables: temperature and CO2 flow. For the cylindrical briquettes, the increase of charcoal (5, 10, 15 wt%) in the coal-charcoal mixtures caused an increase on the bulk density and on the compressive strength of the heat treated briquettes. Above 15 wt% of charcoal in the mixtures, the bulk density and the compressive strength decreased. It was found out that both green and heat treated briquettes had a decrease in compressive strength with the increase of the coal particle size. Optimum results of compressive strength were obtained in the briquettes with 15 wt% of charcoal, particle size <0.044 mm, heat treatment temperature of 1100°C for 8 hours. The increase in charcoal proportion caused an increase in the CO2 reactivity of the briquettes. The SEM micrographs of the heat treated briquettes showed that the texture of the briquettes tend to be more homogeneous with the increase of charcoal in the mixture. The properties of the briquettes produced in the laboratorial briquetting machine showed that a large scale production could be viable. Also, it was found out that the addition of wood charcoal in the mixture directly affects the compressive strength and the CO2 reactivity of the briquettes due to factors such as: the ashes composition, the decrease in fluidity because of the inert material in the mixture, the formation of a porous structure inside the carbon matrix. It was not found a relation between the alkalinity index and the CO2 reactivity in the briquettes.
8

Efeito das principais variáveis do processo de fabricação sobre as propriedades de briquetes de misturas de carvão fóssil e carvão vegetal para uso siderúrgico. / Effect of the main process variables on the proprieties of briquettes of mixtures of coal and charcoal for steelmaking.

Lina Maria Varon Cardona 28 September 2017 (has links)
A utilização de briquetes de misturas de carvão fóssil e biomassa em substituição ao coque como agente redutor pode contribuir para a diminuição das emissões de CO2 à atmosfera no processo de redução de minério de ferro. O fenômeno do amolecimento e fluidificação do carvão fóssil durante o aquecimento permite que o mesmo absorva certa quantidade de materiais inertes à coqueificação durante o tratamento térmico. O objetivo deste trabalho é correlacionar o efeito das principais variáveis de processo de fabricação (temperatura e tempo de tratamento térmico, tamanho de partícula dos componentes, porosidade e proporção de carvão vegetal e carvão fóssil) sobre as propriedades obtidas (resistência mecânica e reatividade ao CO2) de briquetes compostos de misturas de carvão fóssil e carvão vegetal, para uso na indústria siderúrgica. Briquetes de dois formatos diferentes foram preparados em matriz cilíndrica e em maquina briquetadeira e tratados termicamente em forno vertical aquecido com resistência elétrica sob atmosfera de nitrogênio. A resistência à compressão dos briquetes foi analisada em função das seguintes variáveis: proporção de carvão fóssil e carvão vegetal, taxa de aquecimento do tratamento térmico e tamanho de partícula dos carvões. A reatividade ao CO2 dos briquetes tratados termicamente foi analisada em função das seguintes variáveis: temperatura de ensaio e vazão de CO2. Foram comparados os resultados obtidos de ambos os formatos de briquetes. Com o aumento da proporção de carvão vegetal nos briquetes cilíndricos de biocoque, a densidade aparente e a resistência à compressão após tratamento térmico aumentaram para as misturas contendo 5, 10 e 15% de carvão vegetal. A partir dessa composição (15% de carvão vegetal) tanto a densidade final quanto a resistência à compressão apresentaram diminuição. Encontrou-se que tanto os briquetes cilíndricos a verde quanto os briquetes tratados termicamente apresentam perda de resistência mecânica com o aumento do tamanho de partícula do carvão fóssil. Os melhores valores de resistência à compressão foram obtidos em briquetes feitos com carvão fóssil em mistura de 15% em peso de carvão vegetal, tamanho de partícula abaixo de 0,044 mm, tratados termicamente a 1100°C durante 8 horas. Com o aumento na adição de carvão vegetal nos briquetes compostos de carvão fóssil e carvão vegetal, observou-se um aumento da reatividade do biocoque ao CO2. As micrografias dos briquetes tratados termicamente mostraram que a textura dos briquetes tende a ser mais homogênea com aumento de carvão vegetal de madeira na mistura. Os briquetes de biocoque fabricados em briquetadeira permitiram a ampliação do processo de fabricação de briquetes a uma escala laboratorial maior e mostraram a viabilidade industrial na fabricação do biocoque. Encontrou-se que a adição de carvão vegetal de madeira na mistura influencia diretamente na resistência a compressão e a reatividade ao CO2, devido a diferentes fatores como a composição das cinzas da madeira, a diminuição da fluidez devido à ação do inerte na mistura a carbonizar, a formação de uma estrutura porosa dentro da matriz carbonosa. Não encontrou-se correlação entre o índice de alcalinidade dos briquetes e sua reatividade ao CO2. / The substitution of metallurgical coke by briquetted mixtures of coal and biomass as a reducing agent can lower the emissions of greenhouse gases (CO2) in the iron and steelmaking industry. The thermal plasticity of the coking coal can be used to absorb an amount of inert materials during heat treatment. The objective of this study is to correlate the effect of the main processes variables (heat treatment temperature and duration, particle size of the materials, porosity and coal and charcoal ratio) on the properties (compressive strength and CO2 reactivity) of briquetted mixtures of coal and charcoal. Two types of briquettes were produced, one in a cylindrical die and another in a laboratory briquetting machine. The briquettes were heat treated in a vertical electrical furnace under nitrogen atmosphere. The compressive strength of the briquettes was analyzed as a function of the following variables: coal and charcoal ratio, heating rate and particle size. The CO2 reactivity of the heat treated briquettes was analyzed as a function of the following variables: temperature and CO2 flow. For the cylindrical briquettes, the increase of charcoal (5, 10, 15 wt%) in the coal-charcoal mixtures caused an increase on the bulk density and on the compressive strength of the heat treated briquettes. Above 15 wt% of charcoal in the mixtures, the bulk density and the compressive strength decreased. It was found out that both green and heat treated briquettes had a decrease in compressive strength with the increase of the coal particle size. Optimum results of compressive strength were obtained in the briquettes with 15 wt% of charcoal, particle size <0.044 mm, heat treatment temperature of 1100°C for 8 hours. The increase in charcoal proportion caused an increase in the CO2 reactivity of the briquettes. The SEM micrographs of the heat treated briquettes showed that the texture of the briquettes tend to be more homogeneous with the increase of charcoal in the mixture. The properties of the briquettes produced in the laboratorial briquetting machine showed that a large scale production could be viable. Also, it was found out that the addition of wood charcoal in the mixture directly affects the compressive strength and the CO2 reactivity of the briquettes due to factors such as: the ashes composition, the decrease in fluidity because of the inert material in the mixture, the formation of a porous structure inside the carbon matrix. It was not found a relation between the alkalinity index and the CO2 reactivity in the briquettes.
9

Brown coal char CO2-gasification kinetics with respect to the char structure

Komarova, Evgeniia 11 September 2017 (has links) (PDF)
This research has been performed in the framework of the Virtuhcon project, which intends to virtualize high temperature conversion processes. Coal gasification is one of these processes, which is nowadays considered as a promising technology for the chemical industry. This study is devoted to the coal char physical structure, which is one of the most important parameters influencing coal gasification reaction. First, this study presents the extensive literature review of the char physical structure role during its conversion. Collection of the char structural properties as well as their changes during char conversion are shown and discussed. Literature review is followed by the experimental investigations. Chars prepared from two brown coals (Lusatian and Rhenish) were gasified in a laboratory scale fluidized bed reactor in CO2 at temperatures of 800, 850, 900, and 950 °C and atmospheric pressure. Char samples were gasified completely as well as partially in order to evaluate the reaction kinetics and char structural changes during the reaction, respectively. Complete gasification curves were evaluated by different methods, including application of three gasification models (the Random Pore Model, the Volume Reaction Model, and the Shrinking Reaction Model), instantaneous reaction rate approach as well as the self-developed surface-related reaction rate approach. The results of different approaches were compared. This study also presents a comprehensive methodology to analyze coal char physical structure. The variety of measurement techniques (gas physical adsorption, mercury porosimetry, helium pycnometry, SEM, etc.) were applied to assess structural properties of the char, such as specific surface area, particle density, porosity, pore size and shape, structure morphology, etc. Problems associated with the choice of a proper measurement technique and the comparability of the data delivered by different techniques were discussed. The main objective of the study was to link char structural changes to the char gasification kinetics. The specific task of this thesis was to investigate pore size in relation to their availability for the reaction. As such, specific surface areas of pores of different sizes (from sub-micro to mesopores) were correlated to the instantaneous reaction rates. Both chars exhibit similar trends in their structural changes during gasification, although the absolute values differ, especially with respect to the pores of microscale. Furthermore, structural changes were caused not only by the reaction but also by the influence of the heat treatment, especially at the earlier stages of the reaction. The most reasonable correlation has been achieved between the instantaneous reaction rate and the specific surface area of mesopores. Sub-micro- and micropores did not govern the gasification reaction under given conditions. Finally, kinetic parameters derived from different evaluation methods were reapplied in order to test their ability to predict the experimental data. Each of the method has its advantages and disadvantages as used for the kinetic evaluation. The results of this study represent a substantive base of the experimentally derived data concerning physical structure and morphology of coal char. The findings can be used in numerical and simulation studies for development, validation, and improvement of the models which consider coal particle as a reactive porous solid.
10

Brown coal char CO2-gasification kinetics with respect to the char structure

Komarova, Evgeniia 14 August 2017 (has links)
This research has been performed in the framework of the Virtuhcon project, which intends to virtualize high temperature conversion processes. Coal gasification is one of these processes, which is nowadays considered as a promising technology for the chemical industry. This study is devoted to the coal char physical structure, which is one of the most important parameters influencing coal gasification reaction. First, this study presents the extensive literature review of the char physical structure role during its conversion. Collection of the char structural properties as well as their changes during char conversion are shown and discussed. Literature review is followed by the experimental investigations. Chars prepared from two brown coals (Lusatian and Rhenish) were gasified in a laboratory scale fluidized bed reactor in CO2 at temperatures of 800, 850, 900, and 950 °C and atmospheric pressure. Char samples were gasified completely as well as partially in order to evaluate the reaction kinetics and char structural changes during the reaction, respectively. Complete gasification curves were evaluated by different methods, including application of three gasification models (the Random Pore Model, the Volume Reaction Model, and the Shrinking Reaction Model), instantaneous reaction rate approach as well as the self-developed surface-related reaction rate approach. The results of different approaches were compared. This study also presents a comprehensive methodology to analyze coal char physical structure. The variety of measurement techniques (gas physical adsorption, mercury porosimetry, helium pycnometry, SEM, etc.) were applied to assess structural properties of the char, such as specific surface area, particle density, porosity, pore size and shape, structure morphology, etc. Problems associated with the choice of a proper measurement technique and the comparability of the data delivered by different techniques were discussed. The main objective of the study was to link char structural changes to the char gasification kinetics. The specific task of this thesis was to investigate pore size in relation to their availability for the reaction. As such, specific surface areas of pores of different sizes (from sub-micro to mesopores) were correlated to the instantaneous reaction rates. Both chars exhibit similar trends in their structural changes during gasification, although the absolute values differ, especially with respect to the pores of microscale. Furthermore, structural changes were caused not only by the reaction but also by the influence of the heat treatment, especially at the earlier stages of the reaction. The most reasonable correlation has been achieved between the instantaneous reaction rate and the specific surface area of mesopores. Sub-micro- and micropores did not govern the gasification reaction under given conditions. Finally, kinetic parameters derived from different evaluation methods were reapplied in order to test their ability to predict the experimental data. Each of the method has its advantages and disadvantages as used for the kinetic evaluation. The results of this study represent a substantive base of the experimentally derived data concerning physical structure and morphology of coal char. The findings can be used in numerical and simulation studies for development, validation, and improvement of the models which consider coal particle as a reactive porous solid.

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