Lithium interaction with nitrogen molecules trapped in defective multilayer graphene

IF 6.3 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Applied Surface Science Pub Date : 2025-04-05 DOI:10.1016/j.apsusc.2025.163150

K.M. Popov, V.I. Sysoev, Y.V. Fedoseeva, A.A. Makarova, L.G. Bulusheva, A.V. Okotrub

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Abstract

Effect of carbon on the interaction of lithium with highly stable nitrogen molecule requires study for practical use in energy storage and electrochemical nitrogen reduction. In this work, we consider the interaction of lithium with nitrogen molecules embedded in defective multilayer graphene using synchrotron X-ray spectroscopy. Multilayer graphene synthesized by chemical vapor deposition was bombarded with 1 keV nitrogen ions to create lattice defects and insert ∼10 at.% nitrogen, and then used for lithium vapor deposition. All modifications of the graphene sample were carried under ultra-high vacuum conditions and accompanied by measurements of X-ray photoelectron and near-edge X-ray absorption fine structure spectra. Analysis of the spectra revealed the formation of intercalated N₂ molecules as a result of bombardment of graphene and their covalent interaction with deposited lithium. According to density functional theory calculations, the valence orbitals of N₂ and Li hybridize with the π-orbitals of graphene, which increases the bonding between the intercalants. This finding provides new insights into the processes occurring in N₂-intercalated graphene-based electrode materials during lithiation and can be used to develop efficient lithium-based electrochemical energy storage systems and electrochemical approaches for N₂ reduction reaction.

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碳对锂与高度稳定的氮分子相互作用的影响需要研究，以便实际应用于能量存储和电化学氮还原。在这项工作中，我们使用同步辐射 X 射线光谱法研究了锂与嵌入缺陷多层石墨烯中的氮分子的相互作用。用 1 keV 氮离子轰击化学气相沉积合成的多层石墨烯，以产生晶格缺陷并插入 ∼10 at.% 的氮，然后用于锂气相沉积。石墨烯样品的所有改性都是在超高真空条件下进行的，同时还测量了 X 射线光电子和近边 X 射线吸收精细结构光谱。光谱分析显示，由于石墨烯受到轰击，形成了插层 N2 分子，这些分子与沉积的锂发生了共价作用。根据密度泛函理论计算，N2 和锂的价轨道与石墨烯的π轨道杂化，从而增加了插层物之间的键合。这一发现为锂化过程中发生在 N2 嵌入石墨烯基电极材料中的过程提供了新的见解，可用于开发高效的锂基电化学储能系统和 N2 还原反应的电化学方法。

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来源期刊

Applied Surface Science 工程技术-材料科学：膜

CiteScore

12.50

自引率

7.50%

发文量

3393

审稿时长

67 days

期刊介绍： Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.