The self-assembled monolayer (SAM) technique, known for its customizable molecular segments and active end groups, is widely recognized as a powerful tool for regulating the interfacial properties of high-energy-density lithium metal batteries. However, it remains unclear how the degree of long-range order in SAMs affects the solid electrolyte interphase (SEI). In this study, we precisely controlled the hydrolysis of silanes to construct monolayers with varying degrees of long-range order and investigated their effects on the SEI nanostructure and lithium anode performance. The results indicate that the degree of long-range order in SAMs significantly influences the decomposition kinetics of the carbon–fluorine bond in lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), promoting the formation of a LiF-rich SEI and profoundly affecting the long-term stability of the highly sensitive anode during electrochemical processes. These findings provide new insights and directions for the molecular design of SAMs tailored for long-lasting lithium metal interfaces.

中文翻译：

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确定界面长程有序在调节锂金属电池中固体电解质界面中的作用


自组装单层 （SAM） 技术以其可定制的分子片段和活性端基而闻名，被广泛认为是调节高能量密度锂金属电池界面特性的有力工具。然而，目前尚不清楚 SAM 中的长程有序程度如何影响固体电解质界面 （SEI）。在这项研究中，我们精确控制硅烷的水解以构建具有不同程度长程有序的单分子层，并研究了它们对 SEI 纳米结构和锂负极性能的影响。结果表明，SAMs中长程有序程度显著影响双（三氟甲烷磺酰基）酰亚胺锂（LiTFSI）中碳氟键的分解动力学，促进富含LiF的SEI的形成，并深刻影响高灵敏度负极在电化学过程中的长期稳定性。这些发现为为长效锂金属界面量身定制的 SAM 的分子设计提供了新的见解和方向。