Yu Jiangang, Liu Lili, Li Quansheng, Xu Zhidong, Shi Yujia, Lei Cheng
State Key Laboratory of Exterme Environment Optoelectronic Dynamic Measyrement Technology and Instrument, North University of China, Taiyuan 030051, China.
Molecules. 2025 Jul 31;30(15):3223. doi: 10.3390/molecules30153223.
Hydrogen energy holds immense potential to address the global energy crisis and environmental challenges. However, its large-scale application is severely hindered by the lack of efficient hydrogen storage materials. This study systematically investigates the H adsorption properties of intrinsic C fullerene and Li-decorated C fullerene using density functional theory (DFT) calculations. The results reveal that Li atoms preferentially bind to the H site of C, driven by significant electron transfer (0.90 |e|) from Li to C. This electron redistribution modulates the electronic structure of C, as evidenced by projected density of states (PDOS) analysis, where the p orbitals of C atoms near the Fermi level undergo hybridization with Li orbitals, enhancing the electrostatic environment for H adsorption. For Li-decorated C, the average adsorption energy and consecutive adsorption energy decrease as more H molecules are adsorbed, indicating a gradual weakening of adsorption strength and signifying a saturation limit of three H molecules. Charge density difference and PDOS analyses further demonstrate that H adsorption induces synergistic electron transfer from both Li (0.89 |e| loss) and H (0.01 |e| loss) to C (0.90 |e| gain), with orbital hybridization between H s orbitals, C p orbitals, and Li orbitals stabilizing the adsorbed system. This study aimed to provide a comprehensive understanding of the microscopic mechanism underlying Li-enhanced H adsorption on C fullerene and offer insights into the rational design of metal-decorated fullerene-based systems for efficient hydrogen storage.
氢能在应对全球能源危机和环境挑战方面具有巨大潜力。然而，高效储氢材料的缺乏严重阻碍了其大规模应用。本研究使用密度泛函理论（DFT）计算系统地研究了本征C富勒烯和锂修饰C富勒烯的H吸附特性。结果表明，由于从Li到C的显著电子转移（0.90 |e|），Li原子优先与C的H位点结合。这种电子重新分布调节了C的电子结构，态密度投影（PDOS）分析证明了这一点，其中费米能级附近C原子的p轨道与Li轨道发生杂化，增强了H吸附的静电环境。对于锂修饰的C，随着更多H分子被吸附，平均吸附能和连续吸附能降低，表明吸附强度逐渐减弱，意味着三个H分子的饱和极限。电荷密度差和PDOS分析进一步表明，H吸附诱导了从Li（损失0.89 |e|）和H（损失0.01 |e|）到C（获得0.90 |e|）的协同电子转移，H s轨道、C p轨道和Li轨道之间的轨道杂化稳定了吸附体系。本研究旨在全面了解锂增强C富勒烯上H吸附的微观机制，并为合理设计基于金属修饰富勒烯的高效储氢系统提供见解。
