The thermal energy required for regeneration of CO2-rich adsorbents or absorbents is usually regarded as the most important criterion to evaluate different materials and processes for application in commercialscale CO2 capture systems. It is expected that the regeneration heat can be greatly reduced by replacing the mature aqueous monoethanolamine (MEA) technology with amine-based solid adsorbents capturing systems, due to the much lower heat capacity of solid adsorbents comparing to aqueous MEA and the avoidance of evaporating a large amount of water in the regenerator. Comparing to the MEA technology, the regeneration heat for solid adsorbent based systems has not received adequate attention especially on the impacts of process related parameters. Further, the methodologies used in previous investigations to calculate the regeneration heat may have deficiencies in defining the working capacities, adopting proper heat recovery strategies and/or evaluating the effect of moisture co-adsorption. In this study, an energy equation to calculate the regeneration heat has been revised and proposed to systematically evaluate the most important parameters affecting the regeneration heat, including the physical properties of the adsorbents and process related variables including the heat of adsorption, specific heat capacity, working capacity, moisture adsorption of the polyethyleneimine (PEI)/silica adsorbent, the swing temperature difference and the degree of heat recovery. Based on the parametric analysis, the calculated regeneration heat for the PEI/silica adsorbent based system is found to be around 2.46 GJ/tCO2, which is much lower than the value of 3.9 GJ/tCO2 for a typical aqueous MEA system and is also lower than 3.3 GJ/tCO2 for an advanced MEA system. Sensitivity analysis of all the parameters has also been conducted and the results have shown that working capacity, moisture adsorption and heat recovery ratios are the most influential factors. With more proficiency and development in the energy efficient process designs, the advantages of a solid adsorbent based capturing system over typical MEA systems will be justified

Carbon Capture and Storage (CCS) uses a combination of technologies to capture, transport and store carbon dioxide (CO2) emissions from large point sources such as coal or natural gas-fired power plants. Capturing CO2 from ambient air has been considered as a carbon-negative technology to mitigate anthropogenic CO2 emissions in the air. The performance of a mesoporous silica-supported polyethyleneimine (PEI)–silica adsorbent for CO2 capture from ambient air has been evaluated in a laboratory-scale Bubbling Fluidized Bed (BFB) reactor. The air capture tests lasted for between 4 and 14 days using 1 kg of the PEI–silica adsorbent in the BFB reactor. Despite the low CO2 concentration in ambient air, nearly 100% CO2 capture efficiency has been achieved with a relatively short gas–solid contact time of 7.5 s. The equilibrium CO2 adsorption capacity for air capture was found to be as high as 7.3 wt%, which is amongst the highest values reported to date. A conceptual design is completed to evaluate the technological and economic feasibility of using PEI–silica adsorbent to capture CO2 from ambient air at a large scale of capturing 1 Mt-CO2 per year. The proposed novel “PEI-CFB air capture system” mainly comprises a Circulating Fluidized Bed (CFB) adsorber and a BFB desorber with a CO2 capture capacity of 40 t-CO2/day. Large pressure drop is required to drive the air through the CFB adsorber and also to suspend and circulate the solid adsorbents within the loop, resulting in higher electricity demand than other reported air capture systems. However, the Temperature Swing Adsorption (TSA) technology adopted for the regeneration strategy in the separate BFB desorber has resulted in much smaller thermal energy requirement. The total energy required is 6.6 GJ/t-CO2 which is comparable to other reference air capture systems. By projecting a future scenario where decarbonization of large point energy sources has been largely implemented by integration of CCS technologies, the operating cost under this scenario is estimated to be $108/t-CO2 captured and $152/t-CO2 avoided with an avoided fraction of 0.71. Further research on the proposed 40 t-CO2/day ‘PEI-CFB Air Capture System’ is still needed which should include the evaluation of the capital costs and the experimental investigation of air capture using a laboratory-scale CFB system with the PEI–silica adsorbent