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Fu et al. In situ Catalytic Transformation SCHEME 2 | Absorbents, CO2 adducts, and the resulting valuable chemicals. Hydrogenation Using Rh-Based Catalysts The first example of CO2 capture and in situ hydrogenation is reported by our group in 2013, in which polyethyleneimine 600 (PEI600) or the combination of PEI600 and ethylene glycol is developed to absorb gaseous CO2, affording the PEI-CO2 or ethylene glycol-CO2 adducts. With RhCl3 ·3H2 O/CyPPh2 as catalyst, the captured CO2 can be in situ transformed to formate (Scheme 6) (Li et al., 2013). Furthermore, direct hydrogenation of ammonium carbamate derived from CO2, e.g., DETA+CO2 − (DETA = diethylenetriamine), ammonium carbonates such as [DBNH] [OCO2 (C2 H4 O)3 H], [DBNH] [OCO2 CH2 OH] (DBN=1,5-diaza bicycle[4.3.0]non-5-ene), is also successfully performed facilitated by this Rh-based catalyst. Notably, a higher reaction rate and better results can be achieved when using the captured CO2 in the form of ammonium carbonates as feedstock than using equivalent free gaseous CO2 or ammonium carbamate, implying CO2 activation upon capture with DBN/PEI and glycol. After that, we further design a tunable ethoxyl-functionalized amidine to absorb CO2 in order to avoid the use of volatile proton donor (Li et al., 2014). As an activated form of CO2, the captured CO2 in the form of zwitterionic amidinium carbonate is further hydrogenated to formate employing RhCl3/DPEphos as the catalyst (Scheme6). In the same time, we find that the CO2 capture product of potassium phthalimide in PEG150, can also be in situ hydrogenated to formic acid catalyzed by RhCl3 ·3H2 O/CyPPh2 (Scheme 6) (Zhang et al., 2014). Hydrogenation Using Ru- and Fe-Based Catalysts Ru-based catalysts are also promising candidates for the hydrogenation of captured CO2. In the study of Yadav et al., CO2 is captured by DBU and an alcohol to form the alkyl carbonate ionic liquid and the resulting alkyl carbonate is hydrogenated into [DBUH+] formate and methyl formate facilitated by RuCl2 (PPh3 )3 (Scheme 7) (Yadav et al., 2014). Although the reactive species (i.e., alkyl carbonates or CO2) cannot be identified at this stage, this result indicates that alkyl carbonates may be a substrate for hydrogenation, in addition to free CO2 . In 2015, Sanford group combined CO2 capture to form a carbamate salt with hydrogenation to generate CH3OH (Rezayee et al., 2015). In their study, NHMe2 is used to capture CO2 and a homogeneous Ru-based catalyst is used to facilitate the hydrogenation of the captured CO2 to a mixture of DMF and CH3OH (Scheme 7). Although the formation of carbamate salt can decrease the eletrophilicity of CO2, causing the captured CO2 difficult to hydrogenate, the existence of the equilibrium between DMC (Dimethylammonium dimethylcarbamate) and Frontiers in Chemistry | www.frontiersin.org 4 July 2019 | Volume 7 | Article 525PDF Image | CO2 Capture and in situ Catalytic Transformation
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