Tachikawa Hiroto, Izumi Yoshiki, Iyama Tetsuji, Abe Shigeaki, Watanabe Ikuya
Department of Applied Chemistry, Graduate School of Engineering, Hokkaido University, Sapporo 060-8628, Japan.
Department of Dental and Biomedical Materials Science, Graduate School of Biomedical Sciences, Nagasaki University, Nagasaki 852-8102, Japan.
Nanomaterials (Basel). 2023 Jul 11;13(14):2046. doi: 10.3390/nano13142046.
Graphene nanoflakes are widely utilized as high-performance molecular devices due to their chemical stability and light weight. In the present study, the interaction of aluminum species with graphene nanoflake (denoted as GR-Al) has been investigated using the density functional theory (DFT) method to elucidate the doping effects of Al metal on the electronic states of GR. The mechanisms of the diffusion of Al on GR surface and the hydrogen storage of GR-Al were also investigated in detail. The neutral, mono-, di-, and trivalent Al ions (expressed as Al, Al, Al, and Al, respectively) were examined as the Al species. The DFT calculations showed that the charge transfer interaction between Al and GR plays an important role in the binding of Al species to GR. The diffusion path of Al on GR surface was determined: the barrier heights of Al diffusion were calculated to be 2.1-2.8 kcal mol, which are lower than Li on GR (7.2 kcal/mol). The possibility of using GR-Al for hydrogen storage was also discussed on the basis of the theoretical results.
由于其化学稳定性和轻质特性，石墨烯纳米片被广泛用作高性能分子器件。在本研究中，利用密度泛函理论（DFT）方法研究了铝物种与石墨烯纳米片（记为GR-Al）的相互作用，以阐明铝金属对GR电子态的掺杂效应。还详细研究了铝在GR表面的扩散机制以及GR-Al的储氢情况。中性、一价、二价和三价铝离子（分别表示为Al、Al、Al和Al）作为铝物种进行了研究。DFT计算表明，铝与GR之间的电荷转移相互作用在铝物种与GR的结合中起着重要作用。确定了铝在GR表面上的扩散路径：计算得出铝扩散的势垒高度为2.1 - 2.8千卡/摩尔，低于锂在GR上的扩散势垒（7.2千卡/摩尔）。还基于理论结果讨论了使用GR-Al进行储氢的可能性。
