Finial Scientific/Technical Report: Application of a Circulating Fluidized Bed Process for the Chemical Looping Combustion of Solid Fuel

Abstract

Chemical Looping Combustion is a novel combustion technology for the inherent separation of the greenhouse gas, CO{sub 2}. In 1983, Richter and Knoche proposed reversible combustion, which utilized both the oxidation and reduction of metal. Metal associated with its oxidized form as an oxygen carrier was circulated between two reactors--oxidizer and reducer. In the reducer, the solid oxygen carrier reacts with the fuel to produce CO{sub 2}, H{sub 2}O and elemental metal only. Pure CO{sub 2} will be obtained in the exit gas stream from the reducer after H{sub 2}O is condensed. The pure CO{sub 2} is ready for subsequent sequestration. In the oxidizer, the elemental metal reacts with air to form metal oxide and separate oxygen from nitrogen. Only nitrogen and some unused oxygen are emitted from the oxidizer. The advantage of CLC compared to normal combustion is that CO{sub 2} is not diluted with nitrogen but obtained in a relatively pure form without any energy needed for separation. In addition to the energy-free purification of CO{sub 2}, the CLC process also provides two other benefits. First, NO{sub x} formation can be largely eliminated. Secondly, the thermal efficiency of a CLC system is very high. Presently, the CLC processmore » has only been used with natural gas. An oxygen carrier based on an energy balance analysis and thermodynamics analysis was selected. Copper (Cu) seems to be the best choice for the CLC system for solid fuels. From this project, the mechanisms of CuO reduction by solid fuels may be as follows: (1) If pyrolysis products of solid fuels are available, reduction of CuO could start at about 400 C or less. (2) If pyrolysis products of solid fuels are unavailable and the reduction temperature is lower, reduction of CuO could occur at an onset temperature of about 500 C, char gasification reactivity in CO{sub 2} was lower at lower temperatures. (3) If pyrolysis products of solid fuels are unavailable and the reduction temperature is higher than 750 C, all reaction reactivities were improved, especially the CO{sub 2} gasification reactivity of char. Thus, the reduction of CuO by the gasification product CO could proceed quickly. Based on the results obtained, the following coal characteristics would be desirable for the Chemical Looping Combustion process: high volatile matter with a high reactivity of the char produced. PRB coal meets these criteria while being comparatively less expensive and also very abundant. The high moisture content present in PRB coal might also increase the reactivity for char gasification through the development of pore structure and specific surface area in the char during pyrolysis. Biomass materials are also suitable, considering the reaction mechanism of CLC system of solid fuels. The feasibility of the chemical looping combustion process of solid fuels was verified by focusing on PRB coal and biomass. Based on PRB coal as the preferred solid fuel in the development of the CLC system, the mass, energy and system in a dual reactor recirculation system has been determined. In the Cu oxidation tests, it was confirmed that the heating rate is the most important effect on the Cu oxidation process. Lower heating rates and lower operational temperatures would result in incomplete conversion of Cu to CuO. Cu{sub 2}O may be the intermediate product. The operating temperature did not affect the reaction rate of the oxidation process. Under any operating conditions, the exothermic properties are clearly shown.« less