Al-Qurashi Ohoud, Soliman Kamal A, Lgaz Hassane, Safi Zaki, Wazzan Nuha
Department of Chemistry, Faculty of Science, University of Jeddah, Jeddah, Saudi Arabia.
Department of Chemistry, Faculty of Science, Benha University, P.O. Box 13518, Benha, Egypt.
J Mol Model. 2024 Nov 18;30(12):405. doi: 10.1007/s00894-024-06198-3.
In recent years, rechargeable batteries have received considerable attention as a way to improve energy storage efficiency. Anodic (negative) electrodes based on Janus two-dimensional (2D) monolayers are among the most promising candidates. In this effort, the adsorption and diffusion of these Li, Na, and Mg ions on and through Janus 2D-TiSSe as anodic material was investigated by means of periodic DFT-D calculations. Electrochemical parameters were computed and compared. The diffusion barrier energies for migration of ions in monolayer TiSSe in three different potential directions were determined. Furthermore, the electronic properties and Mulliken charge analysis and plots of CDD were employed to investigate the interaction between ions and their surrounding surface. Our results show that the adsorption ability of TiSSe surface up to 32 metal ions falls in the following order: Li > Na > Mg. The maximum storage capacity is 337.37 mAh/g for Li/Na ion and 674.75 mAh/g for Mg ion. The average open-circuit voltage is 1.39, 0.93, and 0.73 V for Li, Na, and Mg ions, respectively. Lastly, the minimum diffusion barriers follow the order Li < Na < Mg. The structural, energetic, and thermal stability of clean Janus surface and its saturated adsorbed systems was proved by MD simulations. In addition, we compared the obtained electrochemical parameters to those reported by other researchers. This comprehensive approach demonstrates valuable insights, furthering our understanding of TiSSe's behavior and its suitability for use in MIBs.
DFT calculations were applied with projector augmented plane waves (PAWs)/PBE functional. A two-dimensional (2D) monolayer TiSSe surface was built with a 4 × 4 supercell. The energy cutoff of plane waves was set to 400 eV. The DFT-D3 model has been used to incorporate van der Waals interactions. A geometric relaxation process was conducted using Monhkorst-Pack 8 × 8 × 1 in reciprocal space. The relaxation and electronic calculations were carried out using the Vienna Ab initio Simulation Package (VASP). Using the transition state (TS) search algorithm implemented in the Dmol module, linear synchronous transition and quadratic synchronous transit tools were utilized to find the minimum energy paths.
近年来，可充电电池作为提高能量存储效率的一种方式受到了广泛关注。基于Janus二维（2D）单分子层的阳极（负极）电极是最有前途的候选材料之一。在这项工作中，通过周期性密度泛函理论（DFT）-D计算研究了锂、钠和镁离子在Janus 2D-TiSSe阳极材料上的吸附以及在其中的扩散。计算并比较了电化学参数。确定了离子在单层TiSSe中沿三个不同电势方向迁移的扩散势垒能量。此外，利用电子性质、穆利肯电荷分析和电荷密度差（CDD）图来研究离子与其周围表面之间的相互作用。我们的结果表明，TiSSe表面对多达32种金属离子的吸附能力顺序如下：Li ＞ Na ＞ Mg。Li/Na离子的最大存储容量为337.37 mAh/g，Mg离子的最大存储容量为674.75 mAh/g。Li、Na和Mg离子的平均开路电压分别为1.39、0.93和0.73 V。最后，最小扩散势垒顺序为Li ＜ Na ＜ Mg。分子动力学（MD）模拟证明了清洁Janus表面及其饱和吸附体系的结构、能量和热稳定性。此外，我们将获得的电化学参数与其他研究人员报告的参数进行了比较。这种综合方法展示了有价值的见解，进一步加深了我们对TiSSe行为及其在金属离子电池（MIBs）中应用适用性的理解。
采用投影增强平面波（PAW）/PBE泛函进行DFT计算。用4×4超胞构建二维（2D）单层TiSSe表面。平面波的能量截止设置为400 eV。使用DFT-D3模型来考虑范德华相互作用。在倒易空间中使用Monhkorst-Pack 8×8×1进行几何弛豫过程。使用维也纳从头算模拟包（VASP）进行弛豫和电子计算。利用Dmol模块中实现的过渡态（TS）搜索算法，使用线性同步过渡和二次同步过渡工具来找到最小能量路径。
