The electrode surfaces of degraded lithium-ion batteries (LIB) were analyzed by liquid chromatography-quadrupole time of flight mass spectrometry (LC-QTOF/MS). The solid-electrolyte interphase (SEI) layer influences the performance of LIBs. Therefore, we conducted a study aimed at clarifying the deterioration mechanism of LIBs by examining the components in the SEI before and after degradation due to cycling. We believe that the change in the mass transfer characteristics at the electrode interface influenced by SEI deterioration can be clarified via LC-QTOF/MS, which would allow elucidation of the deterioration mechanism. The analysis results showed that the degradation products contain multiple components, including polymers of carbonate compounds and phosphate esters, which are formed via electrochemical and chemical reactions, resulting in remarkably reduced capacity. Since the invention of lithium-ion batteries (LIB), many research groups have actively conducted research on improving the battery performance.1-7 Excellent properties, including high capacity and high energy density, have been achieved owing to the work conducted so far. As a result, LIBs are not only used as power sources for mobile devices such as phones and personal computers, but are also used as power sources in electric vehicles, aviation, etc., as well as large-scale stationary power sources for smart grids. [8][9][10] Owing to the remarkable expansion in their applications, it is necessary that LIBs are highly durable and safe in various environments; as a result, durability tests for LIBs have been conducted under diverse settings. In addition, the battery deterioration mechanisms in various cases have been widely studied.
11-13To accurately understand the deterioration mechanism, it is necessary to utilize precise mass spectrometry techniques to determine the structure and composition of materials present at the electrode interface, including the electrode surface layer (i.e., solid electrolyte interface or SEI). By conducting a proper structural analysis, the deterioration mechanism can be discussed in terms of the exact reactions occurring at the interface. The chief analytical techniques that are used to structurally analyze the SEI layer include X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR) spectroscopy, and nuclear magnetic resonance spectroscopy (NMR).
14-21All of these techniques enable the estimation of the skeletal structures of the compounds present in the SEI. However, since the structural formula obtained by these techniques is not supported by precise mass information, the exact reactions governing the deterioration mechanism cannot be deduced from these techniques. On the other hand, the use of precise mass spectrometry for analyzing the electrode interface, including the SEI layer, may allow accurate elucidation of the degradation behavior at the electrode interface by distinguishing between the degradation components and the components of the intrinsic SEI layer. Further, methods for suppr...