Jin Yakang, Xue Qingzhong, Zhu Lei, Li Xiaofang, Pan Xinglong, Zhang Jianqiang, Xing Wei, Wu Tiantian, Liu Zilong
State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Qingdao 266580, Shandong, P. R. China.
College of Science, China University of Petroleum, Qingdao 266580, Shandong, P. R. China.
Sci Rep. 2016 May 31;6:26914. doi: 10.1038/srep26914.
With remarkably interesting surface activities, two-dimensional Janus materials arouse intensive interests recently in many fields. We demonstrate by molecular dynamic simulations that hydrofluorinated Janus graphene (J-GN) can self-assemble into Janus nanoscroll (J-NS) at room temperature. The van der Waals (vdW) interaction and the coupling of C-H/π/C-F interaction and π/π interaction are proven to offer the continuous driving force of self-assembly of J-GN. The results show that J-GN can self-assemble into various J-NSs structures, including arcs, multi-wall J-NS and arm-chair-like J-NS by manipulating its original geometry (size and aspect ratio). Moreover, we also investigated self-assembly of hydrofluorinated J-GN and Fe nanowires (NWs), suggesting that Fe NW is a good alternative to activate J-GN to form J-NS. Differently, the strong vdW interaction between J-GN and Fe NW provides the main driving force of the self-assembly. Finally, we studied the hydrogen sorption over the formed J-NS with a considerable interlayer spacing, which reaches the US DOE target, indicating that J-NS is a promising candidate for hydrogen storage by controlling the temperature of system. Our theoretical results firstly provide a versatile route for designing novel J-NS from 2D Janus nanomaterials, which has a great potential application in the realm of hydrogen storage/separation.
二维Janus材料具有引人注目的表面活性，近年来在许多领域引起了广泛关注。我们通过分子动力学模拟证明，氢氟化Janus石墨烯（J-GN）在室温下可以自组装成Janus纳米卷（J-NS）。范德华（vdW）相互作用以及C-H/π/C-F相互作用与π/π相互作用的耦合被证明为J-GN的自组装提供了持续的驱动力。结果表明，通过操纵J-GN的原始几何形状（尺寸和纵横比），它可以自组装成各种J-NS结构，包括弧形、多壁J-NS和扶手椅状J-NS。此外，我们还研究了氢氟化J-GN与铁纳米线（NWs）的自组装，表明铁纳米线是激活J-GN形成J-NS的良好选择。不同的是，J-GN与铁纳米线之间的强vdW相互作用提供了自组装的主要驱动力。最后，我们研究了在具有相当大层间距的形成的J-NS上的氢吸附，其达到了美国能源部的目标，这表明通过控制体系温度，J-NS是一种有前途的储氢候选材料。我们的理论结果首先为从二维Janus纳米材料设计新型J-NS提供了一条通用途径，其在储氢/分离领域具有巨大的潜在应用。
