Aqshat Seth, Sai Spoorti Gattu, K. V. Sai Srinivasan, Ravindran Sujith
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引用次数: 0
摘要
二维材料上的缺陷工程和金属装饰作为一种创造可行的储氢材料的手段,已经获得了极大的关注。这项基于密度泛函理论(DFT)的研究将锂装饰的单空位(SV)和石-威尔士(SW)缺陷硅烯作为通过物理吸附储存氢气的可行介质。缺陷的引入会增加锂原子的结合能,从原始硅烯中的-2.36 eV分别增加到SV和SW硅烯中的-3.44和-2.73 eV,从而阻止锂原子团聚。缺陷和锂金刚体的存在进一步促进了基底对氢气的吸附,结合能在 US-DOE 设定的 -0.2 至 -0.7 eV/H2 之间,测量到的最高结合能为 -0.389 eV/H2。H2 结合能的增强是 Li(p)和 Li(s)轨道与 H(s)轨道共同作用的结果,是硅烯基底向 Li 原子间接电子转移的结果。经双面锂装饰后,两种锂装饰缺陷体系都能有效地存储多个 H2 分子,最高可达 28 H2,最高重力密度为 5.97 wt%。在 300 K 和 310 K 温度下进行的 Ab Initio 分子动力学模拟证实了锂金刚石以及吸附的 H2 分子在室温下的稳定性,并确定了这些系统作为有效、高比重密度、基于物理吸附的储氢介质的可行性。
Enhanced H2 storage in silicene through lithium decoration and single vacancy and Stone-Wales defects: A density functional theory investigation
Defect engineering and metal decoration onto 2-D materials have gained major attention as a means of creating viable hydrogen storage materials. This Density Functional Theory (DFT) based study presents lithium decorated single vacancy (SV) and Stone-Wales (SW) defective silicene as a viable media for storing hydrogen via physisorption. Introducing defects increases the Li adatom's binding energy from −2.36 eV in pristine silicene to −3.44 and −2.73 eV in SV and SW silicene, respectively, preventing Li adatom clustering. The presence of defects and Li adatom further aid hydrogen adsorption onto the substrates with binding energies present between the US-DOE set range of −0.2 to −0.7 eV/H2 with the highest binding energy measured to be −0.389 eV/H2. The enhanced H2 binding energies are a result of a combined contribution of the Li(p) and Li(s) orbitals with the H(s) orbital with an indirect electronic transfer from the silicene substrate to the Li adatom. Upon double side Li decoration, both the Li-decorated defective systems were able to effectively store multiple H2 molecules up to 28 H2 with the highest gravimetric density being 5.97 wt%. Ab Initio molecular dynamic simulations conducted at 300 K and 310 K confirm the stability of the Li adatom as well as the adsorbed H2 molecules at room temperature and establish the viability of these systems as effective, high gravimetric density, physisorption-based hydrogen storage media.