Wu Ruizhe, Wu Sheng, Pan Jie
Collaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by the Province and Ministry, Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules, College of Chemistry and Chemical Engineering, Hubei University, Wuhan, 430062, P. R. China.
MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter, Shaanxi Province Key Laboratory of Advanced Materials and Mesoscopic Physics, School of Physics, Xi'an Jiaotong University, Xi'an, 710049, P. R. China.
Small. 2025 Feb;21(8):e2408986. doi: 10.1002/smll.202408986. Epub 2025 Jan 15.
Owing to the nanoscale thickness, excellent mechanical and chemical stabilities, 2D materials including graphene and hexagonal boron nitride have emerged as promising artificial solid electrolyte interphase (SEI) candidates for lithium metal batteries. However, whether the implementation of 2D materials is beneficial to electrochemical performance remains controversial, and the key to confining the electroplated Li beneath the 2D materials remains elusive. Here, a nanocrystalline graphene (NG) film is synthesized on high-carbon Cu and the Li plating/stripping behavior on Cu grown with different 2D materials is investigated. Interestingly, in contrast to the commonly obtained Li particles on other substrates during nucleation, a smooth Li layer is obtained on NG/Cu, leading to a compact Li layer with more stable electrochemical performance. The finite element method simulations validate that the low electrical conductivity and the high density of defects on NG film drive the fast entry of electrolytes into the NG/Cu interface and promote homogenous Li nucleation. This work reveals the principles of confining electroplated Li beneath the 2D materials, and paves the way for the applications of 2D materials in artificial SEIs and anode-free lithium metal batteries.
由于具有纳米级厚度、出色的机械和化学稳定性，包括石墨烯和六方氮化硼在内的二维材料已成为锂金属电池颇具前景的人工固体电解质界面（SEI）候选材料。然而，二维材料的应用是否有利于电化学性能仍存在争议，并且将电镀锂限制在二维材料之下的关键仍然难以捉摸。在此，在高碳铜上合成了纳米晶石墨烯（NG）薄膜，并研究了在生长有不同二维材料的铜上的锂电镀/剥离行为。有趣的是，与成核过程中在其他基底上通常获得的锂颗粒不同，在NG/铜上获得了光滑的锂层，从而形成了具有更稳定电化学性能的致密锂层。有限元方法模拟证实，NG薄膜的低电导率和高密度缺陷促使电解质快速进入NG/铜界面并促进均匀的锂成核。这项工作揭示了将电镀锂限制在二维材料之下的原理，并为二维材料在人工SEI和无阳极锂金属电池中的应用铺平了道路。
