Graphene functionalization by hydrogen and fluorine has been proposed as a route to modulate its reactivity and electronic properties. However, until now, proposed systems present degradation and limited hydrogen adsorption capacity. In this study, combining first-principles calculations based on density functional theory (DFT) and reactive molecular dynamics, we analyze the tuning of hydrogen adsorption and electronic properties in fluorinated and hydrogenated monolayer graphenes. Our results indicate that fluorine adsorption promotes stronger carbon–hydrogen bonds. By changing the concentration of fluorine and hydrogen, charge density transfer and electronic properties such as the band gap and spin-splitting can be tailored, increasing their potential applicability for electronic and spintronic devices. Despite fluorine not affecting the total H incorporation, the ab initio molecular dynamics results suggest that 3% fluorinated graphene increases hydrogen anchoring, indicating the hydrogenated and fluorinated graphenes potential for hydrogen storage and related applications.

中文翻译：

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从石墨烯到氟代石墨烯调节氢的吸附和电子性质

已经提出了通过氢和氟进行的石墨烯官能化作为调节其反应性和电子性质的途径。然而，直到现在，所提出的系统仍存在降解并限制了氢的吸附能力。在这项研究中，结合基于密度泛函理论（DFT）的第一性原理计算和反应性分子动力学，我们分析了氟化和氢化单层石墨烯中氢吸附和电子性质的调节。我们的结果表明，氟吸附促进了更强的碳氢键。通过改变氟和氢的浓度，可以调整电荷密度转移和电子性能，例如带隙和自旋分裂，从而增加其在电子和自旋电子器件中的潜在适用性。