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Title:Calcium oxide-based sorbents for CO2 capture at high temperature
Author(s):Sayyah, Maryam
Director of Research:Suslick, Kenneth S.
Doctoral Committee Chair(s):Kenis, Paul J.A.
Doctoral Committee Member(s):Suslick, Kenneth S.; Yang, Hong; Flaherty, David W.
Department / Program:Chemical & Biomolecular Engr
Discipline:Chemical Engineering
Degree Granting Institution:University of Illinois at Urbana-Champaign
Degree:Ph.D.
Genre:Dissertation
Subject(s):Calcium Oxide
CO2 capture
Mechanochemistry
Ultrasonic Spray Pyrolysis
Ball Milling
Electrostatic Precipitator
Pre-Combustion
Shrinking Core Model
Abstract:Carbon capture and storage (CCS) has been recognized as a promising approach to mitigate the rapidly increasing amount of CO2 in the atmosphere. The key factor for the advancement of this technology lies in improved and cost-effective capture processes/materials. Pre-combustion CO2 capture from coal-fired power plants is of particular interest in integrated gasification combined cycle (IGCC) design. High concentrations of CO2 and elevated operating pressures/temperatures reduce the energy requirements of this process to 10-16%, which is roughly half that for post-combustion CO2 capture.[1] CaO has emerged as an attractive material to integrate in high temperature CO2 capture processes because of its favorable properties. However, the main drawback of CaO, namely sintering during calcination and thus dramatic decrease in surface area, has questioned its applicability on an industrial scale. To tackle the stability issue of CaO, different strategies have been examined from which incorporation of inert additives into CaO matrix shows great promise. High melting point refractory metal oxides have been identified as an example class of efficient additives. In this dissertation, two less common synthetic approaches, mechanochemistry and ultrasonic spray pyrolysis (USP), were utilized to prepare highly stable CaOcontaining sorbents for CO2 capture. The mechanochemical approach is as an example of top-down synthesis of materials, while spray pyrolysis is considered a bottom-up approach. First, a systematic study on the use of mechanochemistry (e.g., mechanical milling) for preparing CaO-based sorbents is reported. Important parameters such as milling intensity in high energy ball milling equipment, use of process control agent (i.e., wet or dry processing) and milling time were examined, and their effects on the performance and stability of treated CaO sorbents were studied. Next, the first use of ultrasonic spray pyrolysis as a continuous flow method for the facile synthesis of CaO-based materials is discussed. An extensive study of materials’ characterization and CO2 capture performance has been conducted to examine the efficacy of prepared sorbents. Moreover, importance of bottom-up synthetic approach in retaining CO2 capacity is discussed. This work concludes with modeling the sorbent’s performance via a classical shrinking core model to obtain quantitative values of useful parameters for equipment design (e.g., reaction rate constant and diffusivity decay). [1] Eide, L., I.; Bailey, D., W., Capture précombustion. Oil & Gas Science and Technology - Rev. IFP 2005, 60 (3), 475-484
Issue Date:2014-01-16
URI:http://hdl.handle.net/2142/46797
Rights Information:Copyright 2013 Maryam Sayyah
Date Available in IDEALS:2014-01-16
2016-01-16
Date Deposited:2013-12


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