SIMULTANEOUS MECHANICAL AND HEAT ACTIVATION: A NEW ROUTE TO ENHANCE SERPENTINE CARBONATION REACTIVITY AND LOWER CO2 MINERAL SEQUESTRATION PROCESS COST

Coal can support a large fraction of global energy demands for centuries to come, if the environmental problems associated with CO{sub 2} emissions can be overcome. Unlike other candidate technologies, which propose long-term storage (e.g., ocean and geological sequestration), mineral sequestration permanently disposes of CO{sub 2} as geologically stable mineral carbonates. Only benign, naturally occurring materials are formed, eliminating long-term storage and liability issues. Serpentine carbonation is a leading mineral sequestration process candidate, which offers large scale, permanent sequestration. Deposits exceed those needed to carbonate all the CO{sub 2} that could be generated from global coal reserves, and mining and milling costs are reasonable ({approx}$4 to $5/ton). Carbonation is exothermic, providing exciting low-cost process potential. The remaining goal is to develop an economically viable process. An essential step in this development is increasing the carbonation reaction rate and degree of completion, without substantially impacting other process costs. Recently, the Albany Research Center (ARC) has accelerated serpentine carbonation, which occurs naturally over geological time, to near completion in less than an hour. While reaction rates for natural serpentine have been found to be too slow for practical application, both heat and mechanical (attrition grinding) pretreatment were found to substantially enhance carbonation reactivity. Unfortunately, these processes are too energy intensive to be cost-effective in their present form. In this project we explored the potential that utilizing power plant waste heat (e.g., available up to {approx}200-250 C) during mechanical activation (i.e., thermomechanical activation) offers to enhance serpentine mineral carbonation, while reducing pretreatment energy consumption and process cost. This project was carried out in collaboration with the Albany Research Center (ARC) to maximize the insight into the potential thermomechanical activation offers. Lizardite was selected as the model serpentine material for investigation, due to the relative structural simplicity of its lamellar structure when compared with the corrugated and spiral structures of antigorite and chrysotile, respectively. Hot-ground materials were prepared as a function of grinding temperature, time, and intensity. Carbonation reactivity was explored using the standard ARC serpentine carbonation test (155 C, 150 atm CO{sub 2}, and 1 hr). The product feedstock and carbonation materials were investigated via a battery of techniques, including X-ray powder diffraction, electron microscopy, thermogravimetric and differential thermal, BET, elemental, and infrared analysis. The incorporation of low-level heat with moderate mechanical activation (i.e., thermomechanical activation) was found to be able to substantially enhance serpentine carbonation reactivity in comparison with moderate mechanical activation alone. Increases in the extent of carbonation of over 70% have been observed in this feasibility study, indicating thermomechanical activation offers substantial potential to lower process cost. Investigations of the thermomechanically activated materials that formed indicate adding low-level heat during moderately intense lizardite mechanical activation promotes (1) energy absorption during activation, (2) structural disorder, and (3) dehydroxylation, as well as carbonation reactivity, with the level of energy absorption, structural disorder and dehydroxylation generally increasing with increasing activation temperature. Increasing activation temperatures were also associated with decreasing surface areas and water absorptive capacities for the activated product materials. The above decreases in surface area and water absorption capacity can be directly correlated with enhanced particle sintering during thermomechanical activation, as evidenced by electron microscopy observation. The level of induced structural disorder appears to be a key parameter in enhancing carbonation reactivity. However, particle sintering may contribute to reduced reactivity. The effectiveness of thermomechanical activation at enhancing carbonation reactivity appears to be a complicated function of a variety of process parameters, including grinding intensity, feedstock-to-media ratio, time, temperature, etc