Praveer Nishant, Sahoo Rakesh K, Sahu Sridhar
Computational Materials Research Lab, Department of Physics, Indian Institute of Technology (Indian School of Mines), Dhanbad, India.
Department of Materials Science and Engineering, Technion-Israel Institute of Technology, 3200003, Haifa, Israel.
J Mol Model. 2024 Dec 30;31(1):31. doi: 10.1007/s00894-024-06260-0.
Hydrogen storage in porous nanostructured compounds have recently attracted a lot of attention due to the fact that the underlying adsorption mechanism and thermodynamics provide suitable platform for room temperature adsorption and desorption of H molecules. This work reports the findings of a study on the reversible hydrogen storage capacities of Sc and Y decorated C fullerene, conducted using dispersion-corrected density functional theory (DFT) calculation. The transition metal (TM) atoms, such as Sc and Y, are identified to attach to the C-C bridge position of the C fullerene through non-covalent closed-shell interactions. This suggests that the interaction between the TM atoms and the fullerene occurs via weak van der Waals forces rather than stronger covalent bonds. The thermodynamic stability of the decorated fullerene structures is assessed using different reactivity descriptors. Each Sc and Y atom attached to the C fullerene is capable of absorbing maximum of 6 and 7 numbers of hydrogen molecules, respectively. This results in practical gravimetric densities of up to 4.0 wt% and 4.04 wt% at a temperature of 300 K and a pressure of 60 bar. These findings highlight the significant hydrogen storage capacities of the decorated fullerene structures, indicating their potential for practical use in hydrogen storage systems. The average adsorption energy of H molecules is found lying in the range of 0.332-0.276 eV implying the adsorption process to be physisorptive. Overall, the study provides valuable insights into the hydrogen storage capabilities of Sc and Y decorated C fullerene complexes, offering a promising avenue for the development of efficient and reversible hydrogen storage materials for clean energy applications.
Geometry optimization and other electronic structure calculations was performed by Gaussian 09 software using density functional theory (DFT) with the B3LYP-D3 and M06-2X functionals and the basis set 6-311 + G(d,p). The dispersion-corrected and hybrid meta-exchange correlation functionals were employed because of their accuracy in describing non-covalent interactions, rendering them appropriate for investigating hydrogen adsorption on surfaces.
由于潜在的吸附机制和热力学为氢分子在室温下的吸附和解吸提供了合适的平台，多孔纳米结构化合物中的氢存储最近引起了广泛关注。这项工作报告了一项使用色散校正密度泛函理论（DFT）计算对钪（Sc）和钇（Y）修饰的C富勒烯的可逆储氢容量进行研究的结果。过渡金属（TM）原子，如Sc和Y，被确定通过非共价闭壳相互作用附着在C富勒烯的C-C桥位置。这表明TM原子与富勒烯之间的相互作用是通过弱范德华力而非更强的共价键发生的。使用不同的反应性描述符评估修饰富勒烯结构的热力学稳定性。附着在C富勒烯上的每个Sc和Y原子分别能够吸收最多6个和7个氢分子。在300 K温度和60 bar压力下，这导致实际重量密度分别高达4.0 wt%和4.04 wt%。这些发现突出了修饰富勒烯结构显著的储氢容量，表明它们在储氢系统中的实际应用潜力。发现氢分子的平均吸附能在0.332 - 0.276 eV范围内，这意味着吸附过程是物理吸附。总体而言，该研究为Sc和Y修饰的C富勒烯配合物的储氢能力提供了有价值的见解，为开发用于清洁能源应用的高效可逆储氢材料提供了一条有前景的途径。
使用密度泛函理论（DFT），采用B3LYP-D3和M06-2X泛函以及6-311+G(d,p)基组，通过高斯09软件进行几何优化和其他电子结构计算。采用色散校正和混合元交换相关泛函是因为它们在描述非共价相互作用方面的准确性，使其适合研究表面上的氢吸附。
