Reversible hydrogen storage of light transition metal-functionalized C9N4 monolayers under ambient conditions

IF 5.9 3区材料科学 Q2 CHEMISTRY, PHYSICAL

FlatChem Pub Date : 2025-06-17 DOI:10.1016/j.flatc.2025.100902

Naseer H. Kadhim , Hyeonhu Bae , Tanveer Hussain , Heider A. Abdulhussein

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引用次数: 0

Abstract

Driven by the potential of hydrogen (H₂) as a sustainable alternative to conventional energy sources, we have conducted spin-polarized density functional theory (DFT) calculations to examine the viability of a two-dimensional porous C₉N₄ monolayer as an efficient H₂ storage material. Our findings reveal that the adsorption energy of H₂ molecules on the pristine C₉N₄ is insufficient for effective storage. However, when the C₉N₄ monolayer is decorated with selected light transition metals (Sc, Ti, V), the adsorption energy improves significantly. We find that a 2 × 2 supercell of C₉N₄ can accommodate a maximum of four dopants of Sc, Ti and V. The resulting TMs-decorated C₉N₄ structure (TMs@C₉N₄) can adsorb up to 28 H₂ molecules, with average adsorption energies of −0.245, −0.337, and − 0.320 eV of the systems 4Sc@C₉N₄, 4Ti@C₉N₄, and 4 V@C₉N₄, respectively, satisfying the targets set by the US Department of Energy (DOE). Additionally, the gravimetric H₂ densities reach 9.93, 9.72 and 9.52 wt% for 4Sc@C₉N₄, 4Ti@C₉N₄, and 4 V@C₉N₄, respectively. Furthermore, electronic and magnetic analyses indicate that TMs@C₉N₄ has the potential to serve as a superior candidate for energy storage applications. Finally, we explore the H₂ storage at practical conditions of pressure and temperature using the Langmuir-adsorption model.

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常温条件下轻过渡金属功能化C9N4单层膜的可逆储氢

由于氢（H2）作为传统能源的可持续替代品的潜力，我们进行了自旋极化密度泛函理论（DFT）计算，以检验二维多孔C₉N₄单层作为高效储氢材料的可行性。我们的研究结果表明，H2分子在原始C9N4上的吸附能不足以有效储存。然而，当C9N4单层被选择的轻过渡金属（Sc, Ti， V）修饰时，吸附能显著提高。我们发现一个2 × 2的C9N4超级单体可以容纳最多4种Sc、Ti和v的掺杂剂。所得到的tms修饰的C9N4结构（TMs@C9N4）可以吸附多达28个H2分子，系统4Sc@C9N4、4Ti@C9N4和4 V@C9N4的平均吸附能分别为- 0.245、- 0.337和- 0.320 eV，满足美国能源部（DOE）设定的目标。此外，4Sc@C9N4、4Ti@C9N4和4 V@C9N4的重量H2密度分别达到9.93、9.72和9.52 wt%。此外，电子和磁性分析表明，TMs@C9N4具有作为储能应用的优越候选者的潜力。最后，我们利用langmuir -吸附模型探讨了H2在实际压力和温度条件下的储存。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

FlatChem Multiple-

CiteScore

8.40

自引率

6.50%

发文量

104

审稿时长

26 days

期刊介绍： FlatChem - Chemistry of Flat Materials, a new voice in the community, publishes original and significant, cutting-edge research related to the chemistry of graphene and related 2D & layered materials. The overall aim of the journal is to combine the chemistry and applications of these materials, where the submission of communications, full papers, and concepts should contain chemistry in a materials context, which can be both experimental and/or theoretical. In addition to original research articles, FlatChem also offers reviews, minireviews, highlights and perspectives on the future of this research area with the scientific leaders in fields related to Flat Materials. Topics of interest include, but are not limited to, the following: -Design, synthesis, applications and investigation of graphene, graphene related materials and other 2D & layered materials (for example Silicene, Germanene, Phosphorene, MXenes, Boron nitride, Transition metal dichalcogenides) -Characterization of these materials using all forms of spectroscopy and microscopy techniques -Chemical modification or functionalization and dispersion of these materials, as well as interactions with other materials -Exploring the surface chemistry of these materials for applications in: Sensors or detectors in electrochemical/Lab on a Chip devices, Composite materials, Membranes, Environment technology, Catalysis for energy storage and conversion (for example fuel cells, supercapacitors, batteries, hydrogen storage), Biomedical technology (drug delivery, biosensing, bioimaging)