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Figure 18. Au nanoparticles are deposited into shallow nanowells in 2D nanoparticle clusters using SC CO2. Reprinted from reference [75]. Copyright 2016, American Chemical Society. 3. Conclusions and Perspectives In the past few years, 2D nanomaterials with various unprecedented properties have been achieved extensive attention and rapid develop- ment. In this review, we have highlighted the application of SC CO2 technique on materials synthesis and processing, which have many advantages containing environmental friendly, processing simplicity, and capability of preparing controlled nanostructures. They have suc- cessfully exfoliated a variety of 2D layered materials such as graphite, h- BN, TMDs including MoS2 and WS2, and TMOs including MoO3 and WO3. All of these exfoliated nanosheets have ultrathin thickness and defect-free structure. In addition, with the aid of SC CO2, phase engi- neering of TMDs as well as 2D heterostructures constructed using ultra- thin 2D nanomaterials as promising building blocks can also be realized easily. Although the SC CO2 technique displays great promise, the relative low yield and the unclear specific reaction mechanism limit the general application of this strategy. As to the former, the yield of the product is not enough for practical applications even though it is higher than that of traditional solution methods. Thus, the according technology need to be further improved. While for the latter, beyond the basic physical and chemical properties of SC CO2, there are few detailed explanations or mechanism on the typical effect, such as enhanced straining effect on 2D materials. To better and in-depth understand the mechanism, lots of contrast experiments, advanced characterization techniques, and theoretical calculation should be com- bined together in the subsequent studies. As an advanced green chemistry technology, SC CO2 has many opportunities, and ongoing interest in the development of material syn- thesis and processing is constantly being arisen. Considering the effec- tively exfoliation of graphite, h-BN, and MoS2, more 2D nanomaterials with similar layered structure features can be studied with the assistance of SC CO2 in future study. Depending on the particular properties, another potential field ready to explore is the synthesis of new 2D materials, such as metal-organic frameworks (MOFs), metals, and MXenes. Besides, new ultrathin 2D multinary layered nanomaterials including 2D heterostructures, alloyed 2D nanomaterials, and heteroa- tom-doped 2D nanomaterials with great potential applications are also an important future research direction. Therefore, the highlighted SC CO2 technique employed in the current state of research of materials synthesis and processing will encourage readers to explore new oppor- tunities, and more effort should be devoted in this exciting and emerg- ing field for peoples’ health and the sustainable development. Acknowledgements We are grateful to the National Natural Science Foundation of China (No. 21773216, 51173170, 21633015, 21571157), the financial support from the Innova- tion Talents Award of Henan Province (114200510019), and the Key Program of Science and Technology (121PZDGG213) from Zhengzhou Bureau of Science and Technology. Conflict of Interest The authors declare no conflict of interest. Keywords green chemistry, preparation and processing, supercritical carbon dioxide, two-dimensional nanomaterials Energy Environ. 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Rev. 2015, 44, 2702. H. Wang, F. C. Liu, Z. Y. Fang, W. Zhou, Z. Liu, Nanoscale 2014, 6, 12250. Y.F.Yu,S.Hu,L.Q.Su,L.J.Huang,Y.Liu,Z.H.Jin,A.A.Purezky,D. B. Geohegan, K. W. Kim, Y. Zhang, L. Y. Cao, Nano Lett. 2015, 15, 486. Q. P. Lu, Y. F. Yu, Q. L. Ma, B. Chen, H. Zhang, Adv. Mater. 2016, 28, 1917. G. Zhao, S. Han, A. Z. Wang, Y. Z. Wu, M. W. Zhao, Z. P. Wang, X. P. Hao, Adv. Funct. Mater. 2015, 25, 5292. R. A. Sheldon, Green Chem. 2014, 16, 950. R. A. Sheldon, Green Chem. 2005, 7, 267. X. X. Zhang, S. Heinonen, E. Levanen, RSC Adv. 2014, 4, 61137. J. Zhang, Q. K. Zhang, H. Bai, L. Li, J. Li, Chem. Soc. Rev. 2014, 43, 6938. R. H. Sui, P. Charpentier, Chem. Rev. 2012, 112, 3057.PDF Image | CO2 and 2-Dimensional Nanomaterials with Green Chemistry
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