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Molecules 2019, 24, 182 34 of 41 Gratifyingly, encouraging advances on the development of novel strategies to construct organic molecules through C-N bond formation have been made, however, many problems and challenges still remain. Firstly, in most transformations involving CO2 conversion, the catalytic performance in transition metal systems is much better than that of organocatalysis strategies. Generally, the metal complexes easily forming active sites are more beneficial for activating the substrates such as alkene, alkyne and H2, etc. As a result, the catalytic efficiency and selectivity show much higher values, together with the lower catalytic loading, faster reaction rates, shorter times, and lower pressures and temperatures. Despite the superiority of metal complexes, their preparation processes are stricter (they are generally sensitive to water and air) and their stability is lower than that of organocatalysts. Also, the catalytic ability of organocatalysts has improved greatly. In addition, almost all of the metal-based catalysts were focused on the transition metals. Accordingly, the number of examples exploring main group metal-catalyzed transformations of CO2 is inadequate. Secondarily, the model products could be generally obtained in excellent yield and selectivity, but the examples of products being directly used as functional target molecules for medicines, natural products, or bioactive polymers, etc. are limited. Thus, the compatibility of catalytic methods in larger molecules bearing with much more complicated functional groups needs more exploration. Furthermore, for CO2 hydrogenation with amines, high yields and selectivities are achieved much easier using hydrosilanes than H2 as hydrogen source. However, the use of hydrosilanes will be lead to a large amount of siloxane by-products. Therefore, from the point of view of sustainable chemistry, the development of benign H2 process would have great significance and the exploration of robust methods for selective and effective catalysis is also essential despite being challenging. Besides, the efficiency of the noble transition metal-based homogenous schemes and metallic oxide-based heterogeneous catalytic systems must be further improved. Last but not least, it is challenging and imperative to discover more available methods and routes to transform CO2 into valuable chemicals with C-N bonds. Funding: This research was funded by the National Natural Science Foundation of China (21602232) and the Natural Science Foundation of Shanxi Province (201701D221057). Conflicts of Interest: The authors declare no conflict of interest. Abbreviations Carbon dioxide (CO2); ionic liquids (ILs); primitive-cubic (pcu); metal-organic framework (MOF); nuclear magnetic resonance (NMR); gas chromatography (GC); high-resolution mass spectrometry (HRMS); N-heterocyclic carbene (NHC); nanoparticles (NPs); diphosphine-borane (DPB); 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU); dimethyl sulfoxide (DMSO); density functional theory (DFT); polyoxometalate (POM); 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD); tetra-n-butylammonium (TBA); cyanuric acid (H3CYA); triethanolamine (TEOA); p-toluenesulfonyl chloride (TsCl); 1,5,7-triazabicylo[4.4.0]dec-5-ene ([TBDH][TFE]); N-methyl-2-pirrolidinone (NMP); 3-amino-1H-1,2,4-triazole (ATriz); 4,7,10-trioxa-1,13- tridecanediamine (TOTDDA); attenuated total reflectance fourier transform infrared spectroscopy (ATR-FTIR); polymethylhydrosiloxane (PMHS); butylammonium fluoride (TBAF); turnover frequency (TOF); polyaniline-functionalized carbon nanotubes (PANI-CNT); N-doped carbons (NCs) References 1. Tuck, C.O.; Pérez, E.; Horváth, I.T.; Sheldon, R.A.; Poliakoff, M. Valorization of biomass: Deriving more value from waste. Science 2012, 337, 695–699. [CrossRef] [PubMed] 2. He, M.; Sun, Y.; Han, B. Green carbon science: Scientific basis for integrating carbon resource processing, utilization, and recycling. Angew. Chem. Int. Ed. 2013, 52, 9620–9633. [CrossRef] [PubMed] 3. Aresta, M.; Dibenedetto, A.; Angelini, A. Catalysis for the valorization of exhaust carbon: From CO2 to chemicals, materials, and fuels. Technological use of CO2. Chem. Rev. 2014, 114, 1709–1742. [CrossRef] [PubMed] 4. Artz, J.; Müller, T.E.; Thenert, K.; Kleinekorte, J.; Meys, R.; Sternberg, A.; Bardow, A.; Leitner, W. Sustainable conversion of carbon dioxide: An integrated review of catalysis and life cycle assessment. Chem. Rev. 2018, 118, 434–504. [CrossRef] [PubMed] 5. Huang, K.; Sun, C.-L.; Shi, Z.-J. Transition-metal-catalyzed C–C bond formation through the fixation of carbon dioxide. Chem. Soc. Rev. 2011, 40, 2435–2452. [CrossRef] [PubMed]PDF Image | Catalytic Conversion of Carbon Dioxide through C-N Bond
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