Advanced carbon capture and storage technologies
- Autores: Agnieszka Lucyna Cwik
- Directores de la Tesis: Ignasi Casanova (dir. tes.), Katarzyna Zarebska (codir. tes.)
- Lectura: En la Universitat Politècnica de Catalunya (UPC) ( España ) en 2019
- Idioma: español
- Tribunal Calificador de la Tesis: Wojciech Suwala (presid.), Adam Smolinski (secret.), Andrés Enrique Idiart Castellano (voc.)
- Programa de doctorado: Programa de Doctorado Erasmus Mundus en Vías Econo-ambientales para Servicios de Energía Sostenible / Environomical Pathways for Sustainable Energy Services por la Universidad Politécnica de Catalunya; Aalto Yliopisto-Aalto University(Finlandia); Akademia Górniczo-Hutnicza(Polonia); Instituto Superior Técnico de Lisboa(Portugal); Kungliga Tekniska Högskolan-The Royal Institute of Technology (Suecia); Politecnico di Torino(Italia); Technische Universiteit Eindhoven-Eindhoven University of Technology(Países Bajos) y École des Mines de Nantes(Francia)
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- Resumen
In this work two research topics are presented: investigation of carbonation reactions of high – calcium waste materials and CO2 storage in coal.
Firstly, sorption capacity of CO2 and CH4 of hard coal and associated sorption-induced expansion of the material was measured. This investigation was maintained in isothermal and non-isothermal conditions. Experiments were done on purpose-design apparatus allowing simultaneous measurement of sorption kinetics and sorption-induced swelling/contraction of coal. Chosen coal sample had higher sorption capacity for CO2 when compare to capacity for CH4..
Next to CO2 storage, the topic of CO2 utilization has been investigated. Carbonation of European high-calcium fly ashes is assessed. The experiments have been done on different fly ashes with content of 5-36% CaO. Complementary, characterization and analysis of fly ash samples has been performed.
Acceleration of carbonation has been explored. Experiments has been done in temperature range between 25 and 290°C, 1-12 bar of CO2, CO2 + H2O and simulated flue gas over reaction times between 2 and 72 hours. Major conclusions of this work is that increasing the temperature and pressure strongly enhances the process of carbonation. Also, addition of water vapor substantially accelerates the process and increase its kinetics.
This thesis reports that maintaining the carbonation process without steam addition leads to effective carbonation conversion. Chemical fixation of CO2 molecules with solid material of fly ash with high content of CaO to produce calcium carbonate is possible. The highest sequestration capacity achieved is 117.7 g CO2/kg fly ash and highest carbonation efficiency obtained is 48%.
The microstructural analysis of fly ash samples showed the evolution of the cenosphere surface according to the carbonation experiments conditions. Different shapes and sizes of calcium carbonate has been detected after carbonation experiments.
The compositional constraints of fly ashes that control reaction with CO2 has been described. It was found that not the bulk content of CaO is the factor controlling the carbonation reaction, but the content of free lime.
Impact on carbonation of two pressure flow systems was assessed: batch and continuous flow, with and without addition of steam. Using he batch treatment with addition of steam gave the highest carbonation efficiency.
Another set of carbonation experiments which has been done was with using simulated flue gas (84% N2, 15% CO2, 1 % H2O) instead of pure CO2 stream, in conditions: 160°C, 6 bar of gas and 2 hours of reaction time. It was concluded that using flue gas instead of pure stream of carbon dioxide lowers the carbonation rate of about 9%.
Final part of this research was to determine the change of free lime content in fly ash samples before and after carbonation. Carbonation reactions lead to substantial decrease of free lime contents in fly ashes. In most cases, the amount of free lime in fly ash after carbonation was compatible with the current EU legislations regarding fly ash incorporation to cement as admixture.
