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for the 2D layer heterostructure can be chosen; then, 2H-WS2/2H- MoS2 as the preferred van der Waals heterojunctions are formed effi- ciently. An enhanced photoelectrochemical activity toward hydrogen evolution could thus be achieved owning to the advantageous heterostructures prepared with the coexistence of vertical WS2/MoS2 and lateral WS2-WO3H2O and 1T-2H MoS2 heterostructures in one materials unit. 2.5. SC CO2-Assisted Construction of Amorphous Materials In contrast to crystalline nanomaterials, amorphous materials with long-range disorder and short-range order properties bring about new opportunities for practical applications. Recently, amorphous TMDs with abundant active edge sites have been considered as efficient cata- lysts for hydrogen evolution reaction (HER).[68,69] To make out the ori- gin of the amorphous molybdenum sulfide (MoS3) catalytic activity, Benck et al.[70] firstly prepared the amorphous MoS3 materials using a scalable wet chemical method and then investigated the origin of the catalytic activity via a series of spectroscopic and electrochemical charac- terization. The experimental results demonstrated that both the inher- ently favorable surface properties of the active molybdenum sulfide phase and the rough nanostructured film morphology contribute to the high HER activity. In addition, amorphous materials with optical spec- tral properties were also investigated recently. Two-dimensional nanomaterials with tunable localized surface plasmon resonances (LSPR) have been reported and aroused wide attention. As a remarkable class of plasmonic materials, they are superior to traditional precious metals. Using a facial and simple strategy with assistance of SC CO2, Liu et al.[71] achieved 2D amor- phous molybdenum oxide (MoO3) nanosheets with enhanced LSPR under illumination (Figure 16). The oxidation of MoS2 nanosheets during the annealing process and the next step of SC CO2-treatment played key roles in preparing the amorphous MoO3 nanosheets. The strain generated from the stronger interaction of CO2 and amor- phous MoO3 could induce the atomic disorder arrangement. The as- prepared amorphous MoO3 nanosheets exhibited adjustable LSPR in the Vis-NIR regions, which could be used to apply in the optical biosensing system. 2.6. SC CO2-Assisted Construction of Other Functional Nanomaterials Supercritical carbon dioxide with its gas-like penetration, liquid-like solvation abilities, and near-zero surface tension is capable of using as reaction media for new functional nanomaterial processing. Li et al.[72] constructed SC-PFFB/GO nanohybrids with the help of SC CO2 (Fig- ure 17). The introduction of SC CO2 could induce the PFFB to crystal- lize on the GO nanosheets instead of forming amorphous structure. And the change of morphology could lead to the fluorescent enhance- ment of the resultant nanohybrids. To uniformly disperse nanoparticles onto the high-surface-energy supporting materials, Meng et al.[73,74] synthesized nickel nanoparticles dotted graphene oxide nanocomposites (ScNi/GO) and Au/graphene oxide nanocomposite (Sc-Au/GO) via facile SC CO2 chemical deposition and reduction route individually, and the obtained nanocomposites could be utilized as efficient lubricant additives. Except for 2D semiconductor nanomaterials, 2D monolayer metal nanoparticle clusters formation in SC CO2 was reported by Wang et al.[75] The 2D gold (Au) nanoparticle clusters deposited on the shal- low nanoscale wells utilizing SC CO2 were shown in Figure 18. Based on the unique properties of SC CO2, the Au nanoparticles could pene- trate and deposit into nanoscale structures, and then, Au nanoparticles clusters with closely packed uniform arrays were obtained. The strategy of SC CO2 deposition provides a new technique to design and prepare robust 2D nanocluster arrays with desired architecture for widely appli- cations. Figure 17. Schematic illustration of fabrication processes of PFFB/GO, SC-PFFB, and SC-PFFB/GO. PFFB, poly [(9-ylidene-{2-tetradecyloxy-5- tetrafluorophthalimide-phenyl}fluorenyl-2,7-diyl)- alt-(1,4-phenyl)]; GO, graphene oxide. Reprinted from reference [72]. Copyright 2015, Elsevier Ltd. Energy Environ. Mater. 2018, 1, 46–60 58 © 2018 Zhengzhou UniversityPDF Image | CO2 and 2-Dimensional Nanomaterials with Green Chemistry
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