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Fu et al. In situ Catalytic Transformation SCHEME 1 | CCU strategy and its importance in carbon cycle. Motivated by these results, we further develop potassium phthalimide as absorbent to realize equimolar CO2 capture in PEG150. Moreover, the obtained product can be used as in situ transcarboxylating reagent to synthesize oxazolidinone derivatives (Scheme 4) (Zhang et al., 2014). Recently, Hu group subtly designs a CCU example (Yu et al., 2016), in which carbamate salts generated from CO2 and primary amines are used as substrates. The captured CO2 not only acts as a reactant but also acts as a protecting reagent for the amine to avoid poisoning of the copper catalyst. By using 5 mol% of CuI as catalyst, carbamate salts can react with aromatic aldehydes and aromatic terminal alkynes, affording the important oxazolidin-2- ones (Scheme 4). Synthesis of β-Oxopropylcarbamates Based on these inspiring results, our group uses ammonium carbamates as surrogates of carbon dioxide and secondary amines in the three-component synthesis of β-oxopropylcarbamates from propargylic alcohols, secondary amines, and CO2. Catalyzed by silver (I) catalyst, ammonium carbamates can react with propargylic alcohols to generate β-oxopropylcarbamates under atmospheric pressure (Scheme 5) (Song et al., 2015). In this example, the substitution of pure CO2 with the captured CO2 can facilitate the reaction running at atmospheric pressures with a broad substrate and reaction application scope. Furthermore, the solid ammonium carbamates are easier to handle and quantify than the volatile amines and gaseous CO2 . The transcarboxylation is an important transformation strategy for the CO2 adducts to valuable chemicals. However, for the CO2 adducts formed by base and CO2, the transcarboxylation is still limited to the substrates including amines, propargylamines and aziridines. Therefore, novel CO2 absorbents and extended substrates are expected to facilitate the application of CO2 adducts as transcarboxylation reagent in CCU strategy. Besides transcarboxylation, the integral transformation of CO2 capture products is another attractive option in CCU strategy, wherein the ammonium carbamates derived from CO2 and amines is a promising raw material. Nevertheless, the integral transformation of ammonium carbamates to valuable chemicals remains sporadic and underexplored. Hopefully, more conversion protocols of ammonium carbamates can be designed based on the reactivity of amine and CO2. CO2 Capture and in situ Hydrogenation CO2 hydrogenation is widely investigated in the CCU strategy because the basic absorbent can react with the resulting formic acid to form formate, thus overcomes the thermodynamic limitation in the hydrogenation of CO2. In the researches on CO2 capture and in situ hydrogenation, both metal-based homogeneous catalysts (containing Rh-, Ru-, and Fe-based catalysts) and heterogeneous catalysts have been investigated. Frontiers in Chemistry | www.frontiersin.org 3 July 2019 | Volume 7 | Article 525PDF Image | CO2 Capture and in situ Catalytic Transformation
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