In this study, the thermal activation of different types of CaO-based sorbents was examined. Pretreatments were performed at different temperatures (800--1300 degrees C) and different durations (6--48 h) using four Canadian limestones. Sieved fractions of the limestones, powders obtained by grinding, and hydroxides produced following multiple carbonation/calcination cycles achieved in a tube furnace were examined. Pretreated samples were evaluated using two types of thermogravimetric reactors/ analyzers. The most important result was that thermal pretreatment could improve sorbent performance. In comparison to the original, pretreated sorbents showed better conversions over a longer series of CO2 cycles. Moreover, in some cases, sorbent activity actually increased with cycle number, and this effectwas especially pronounced for powdered samples preheated at 1000 degrees C. In these experiments, the increase of conversion with cycle number (designated as self-reactivation) after 30 cycles produced samples that were approximately 50% carbonated for the four sorbents examined here, and there appeared to be the potential for additional increase. These results were explained with the newly proposed pore--skeleton model. This model suggests, in addition to changes in the porous structure of the sorbent, that changes in the pore--skeleton produced during pretreatment strongly influence subsequent carbonation/ calcination cycles.

Carbon capture and storage (CCS) has been identified as an urgent, strategic and essential approach to reduce anthropogenic CO2 emissions, and mitigate the severe consequences of climate change. CO2 storage is the last step in the CCS chain and can be implemented mainly through oceanic and underground geological sequestration, and mineral carbonation. This review paper aims to provide state-of-the-art developments in CO2 storage. The review initially discussed the potential options for CO2 storage by highlighting the present status, current challenges and uncertainties associated with further deployment of established approaches (such as storage in saline aquifers and depleted oil and gas reservoirs) and feasibility demonstration of relatively newer storage concepts (such as hydrate storage and CO2-based enhanced geothermal systems). The second part of the review outlined the critical criteria that are necessary for storage site selection, including geological, geothermal, geohazards, hydrodynamic, basin maturity, and economic, societal and environmental factors. In the third section, the focus was on identification of CO2 behaviour within the reservoir during and after injection, namely injection-induced seismicity, potential leakage pathways, and long-term containment complexities associated with CO2-brine-rock interaction. In addition, a detailed review on storage capacity estimation methods based on different geological media and trapping mechanisms was provided. Finally, an overview of major CO2 storage projects, including their overall outcomes, were outlined. This review indicates that although CO2 storage is a technically proven strategy, the discussed challenges need to be addressed in order to accelerate the deployment of the technology. In addition, beside the necessity of technoeconomic aspects, public acceptance of CO2 storage plays a central role in technology deployment, and the current ethical mechanisms need to be further improved.

This study examines steam reactivation of sorbent to improve the reversibility of multiple CaO-CO2 capture cycles. Experiments to obtain spent sorbent were performed in a tube furnace, and reactivation was achieved using steam in a pressurized reactor. Sorbent activity for CO2 capture was then tested in a thermogravimetric analyzer (TGA), in multi-cycle carbonation tests. After reactivation the sorbent had even better characteristics for CO2 capture than that of the natural sorbent. The average carbonation degree over 10 cycles for the reactivated sorbent approached 70%, significantly higher than for the original sorbent (35-40%). This means that the same sorbent may achieve effective CO2 capture over a large number of cycles, in the absence of other phenomena such as attrition. Partially sulfated sorbents may also be reactivated, but hydration itself is also hindered by sulfation.

The carbonation reaction has recently been intensively investigated as a means of CO 2 capture from gas mixtures such as flue gas produced during fossil fuel combustion. Unfortunately, this gas-solid reaction is limited due to formation of the solid product (CaCO 3 ) at the reacting surface and sintering, all of which reduce the carrying capacity of the sorbent. In this work the enhancement of carbonation conversion by means of steam addition to the carbonating gas was studied. Seven limestones of different origin and composition as well as one synthetic sorbent (calcium aluminate pellets) were tested. A thermogravimetric analyzer (TGA) was employed for the carbonation tests at different temperatures (350-800 °C) in a gas mixture containing typically 20% CO 2 and 10 or 20% H 2 O (g) . The samples tested were calcined under an N 2 (800 °C) or CO 2 (950 °C) atmosphere to explore the influence of different levels of sample sintering, and the results obtained were compared with those seen for carbonation in dry (no steam) gas mixtures. The morphology of samples after carbonation under different conditions was examined by a scanning electron microscope (SEM). It was found that carbonation is enhanced by steam, but this is more pronounced at lower temperatures and for more sintered samples. With increasing temperature and carbonation time, the enhancement of carbonation becomes negligible because the conversion reaches a "maximum" value (∼75-80% for samples calcined in N 2 ) even without steam. Carbonation of samples calcined in CO 2 is enhanced at different levels depending on the sorbent tested. The shape of carbonation profiles and morphology of carbonated samples show that steam enhances solid state diffusion and, consequently, conversion during carbonation.

The development of highly efficient CaO-based pellet sorbents, using inexpensive raw materials (limestones) or the spent sorbent from CO2 capture cycles, and commercially available calcium aluminate cements (CA-14, CA-25, Secar 51, and Secar 80), is described here. The pellets were prepared using untreated powdered limestones or their corresponding hydrated limes and were tested for their CO2 capture carrying capacities for 30 carbonation/calcination cycles in a thermogravimetric analyzer (TGA). Their morphology was also investigated by scanning electron microscopy (SEM) and their compositions before and after carbonation/calcination cycleswere determined by X-ray diffraction (XRD). Pellets prepared in this manner showed superior behavior during CO2 capture cycles compared to natural sorbents, with the highest conversions being > 50% after 30 cycles. This improved performance was attributed to the resulting substructure of the sorbent particles, i.e., a porous structure with nanoparticles incorporated. During carbonation/calcination cycles mayenite (Ca12Al14O33) was formed, which is believed to be responsible for the favorable performance of synthetic CaO-based sorbents doped with alumina compounds. An added advantage of the pellets produced here is their superior strength, offering the possibility of using them in fluidized bed combustion (FBC) systems with minimal sorbent loss due to attrition.

Calcium looping (CaL) is a promising technology for the decarbonation of power generation and carbon-intensive (cement, lime and steel) industries. Although CaL has been extensively researched, some issues need to be addressed before the deployment of this technology at commercial scale. One of the important challenges for CaL is decay of sorbent reactivity during capture/regeneration cycles. Numerous techniques have been explored to enhance natural sorbent performance, to create new synthetic sorbents, and to reactivate and re-use deactivated material. This review provides a critical analysis of natural and synthetic sorbents developed for use in CaL. Special attention is given to the suitability of modified materials for utilisation in fluidised-bed systems. Namely, besides requirements for a practical adsorption capacity; a mechanically strong material, resistant to attrition, is required for the fluidised bed CaL operating conditions. However, the main advantage of CaL is that it employs a widely available and inexpensive sorbent. Hence, a compromise must be made between improving the sorbent performance and increasing its cost, which means a relatively practical, scalable, and inexpensive method to enhance sorbent performance, should be found. This is often neglected when developing new materials focusing only on very high adsorption capacity.

Carbon dioxide (CO2) is the major contributor to greenhouse gas (GHG) emissions and the main driver of climate change. Currently, CO2 utilization is increasingly attracting interest in processes like enhanced oil recovery and coal bed methane and it has the potential to be

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