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Dowson and Styring CO2 Butanol a simple energy calculation shows that the absolute maximum energy price that allows CDU fuel production at around €1/L is €105/MWh (readily achievable by most low-carbon generation methods), the real energy price will have to be much lower to account for process inefficiencies and further issues such as the cost of capturing and purifying the CO2 from the waste streams to begin with. The cOsT OF carBOn caPTUre The high cost of capturing carbon dioxide from waste streams is a major challenge for both CDU and CCS strategies. Despite the thermodynamic de-mixing costs being relatively low in flue gas streams (approximately 150–250 MJ/t CO2 depending on concentration), CO2 capture and purification processes have much larger energy costs stemming from the sorption/desorp- tion process. This is evident where an energetic driving force is required for either the sorption of the carbon dioxide, such as in high pressure adsorption and membrane separation, or for the desorption step, such as in amine-based chemisorption or vacuum swing adsorption. This results in a range of energy costs from approximately 1 to 4 GJ/t CO2 with the lower range consisting mainly of immature techniques and the upper range consisting of benchmark amine processes such as monoethan- olamine (Dowson et al., 2016). Further issues associated with the capture processes involve the challenges of retrofitting existing plants and the footprint size of the capture process facility, which must be sited near to the point source, as well as the interac- tions between the sorbent materials and trace gases in the waste stream which are often corrosive or deleterious, especially to the benchmark amine sorbent materials (Uyanga and Idem, 2007; Soosaiprakasam and Veawab, 2008). Furthermore, temperature swing processes such as the benchmark amine-based processes require a substantial amount of waste heat to desorb the captured CO2 which may be available in sufficient quantity for a capture from certain point sources such as power plants although at a high parasitic energy cost (Lin et al., 2016). However, similar waste heat may not be available in industrial manufacturing waste streams, for example. One potential method to avoid these issues is to directly react the low partial pressure CO2 with a reagent that provides a platform for further product generation. This approach has superficial similarities with amine-based chemisorption pro- cesses, in that a new chemical bond is formed with the flue gas CO2. However, such a direct utilization route has the benefit of not requiring large energy expenditure to re-release the CO2 into the gas phase, but instead takes the “capture product” and directly converts it further to form value-added compounds. By necessity, this will require a stoichiometric quantity of the reagent, which must therefore be able to be generated using environmentally benign processes. Previous work carried out by this group has identified orga- nometallics and particularly Grignard reagents as being suitable for the direct conversion of flue gas concentration of CO2 into value-added products such as acetic, terephthalic, and adipic acids (Dowson et al., 2015). The organomagnesium reagent, which was shown to react readily with CO2, even at low partial pressures, can then be regenerated from the by-product mag- nesium dihalide (MgX2). Electrolysis of the dihalide produces magnesium metal and the elemental halogen, which can then either directly halogenate certain hydrocarbons or be “burned” in hydrogen and subsequently reacted with an alcohol to produce the organohalide starting precursor (RX) to the initial Grignard reagent (Figure 3). In this way, the Grignard reactant is “looped” making the overall process akin to post-combustion chemical looping, which is typically carried out using calcium oxide as a reactive capture agent (Blamey et al., 2010). Again, the difference in this case is that the looping process produces a value-added compound containing the captured CO2 rather than low-value CO2 gas, combining both capture and utilization in one step. As a result, the reduced magnesium consumed during the reaction provides the driving force for the overall process, render- ing all other steps exothermic, and readily carried out at ambi- ent pressures and temperatures. The hydrogen-halide burning process in particular is extremely exothermic and can also allow for surplus energy recovery (Group, 2014). The crucial magne- sium electrolysis step, while highly energy intense, is also highly efficient in industrial magnesium production from sea salts. Faradaic efficiencies approaching 90% have been reported, and energy costs may be further reduced if the expensive magnesium chloride drying process can be avoided by using non-aqueous hydrogen halide for the post-Grignard reaction quench step (Polmear, 1999). Naturally, it should be noted that Grignard reagents are highly sensitive to water, requiring that any incoming flue gas stream that supplies the CO2 for the first step in Figure 3 must FigUre 3 | General Grignard CO2 reaction/cycle scheme including Grignard regeneration using alcohols or hydrocarbons as starting reagents. Frontiers in Energy Research | www.frontiersin.org 4 October 2017 | Volume 5 | Article 26PDF Image | Demonstration of CO2 Conversion to Synthetic Transport Fuel
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