Correlative Electrochemical Microscopy for the Elucidation of the Local Ionic and Electronic Properties of the Solid Electrolyte Interphase in Li‐Ion Batteries

Abstract

The solid‐electrolyte interphase (SEI) plays a key role in the stability of lithium‐ion batteries as the SEI prevents the continuous degradation of the electrolyte at the anode. The SEI acts as an insulating layer for electron transfer, still allowing the ionic flux through the layer. We combine the feedback and multi‐frequency alternating‐current modes of scanning electrochemical microscopy (SECM) for the first time to assess quantitatively the local electronic and ionic properties of the SEI varying the SEI formation conditions and the used electrolytes in the field of Li‐ion batteries (LIB). Correlations between the electronic and ionic properties of the resulting SEI on a model Cu electrode demonstrates the unique feasibility of the proposed strategy to provide the two essential properties of an SEI: ionic and electronic conductivity in dependence on the formation conditions, which is anticipated to exhibit a significant impact on the field of LIBs.

Application of Electrochemical Impedance Spectroscopy to Degradation and Aging Research of Lithium-Ion Batteries

“…168 Recently, Santos et al combined feedback and multifrequency alternating-current modes of scanning electrochemical microscopy (SECM) to evaluate quantitatively the local and in situ electronic and ionic properties of SEI in LIBs for the first time, respectively. 169 The method has potential in calculating the critical parameters of SEI, such as resistivity and dielectric permittivity. In summary, although EIS is a proven technique in characterizing the electrical properties of SEI, the thorny issue is to quantitatively assess the thickness evolution of the SEI during battery aging by monitoring impedance change.…”

Intelligent Monitoring for Safety‐Enhanced Lithium‐Ion/Sodium‐Ion Batteries

“…These gap areas with poor contact may lead to the electrode surface being prone to be the sites of the electrolyte decomposition, Li deposition, capacity loss, gas generation, and other undesirable reactions, which may greatly affect the safety of LIBs. [75][76][77][78] Therefore, ultrasonic scanning images is an important "non-destructive testing" technology to study the interface wetting and stable state of electrolyte during battery aging. At the same time, it has d,e) Comparison of the Δλ B changes with dQ/dV from sixth to the tenth cycle for micro-Si and nano-Si electrodes, respectively.…”

“…In this review, the factors that may cause batteries' safety problems are demonstrated from different component levels of the [78] Copyright 2022, Wiley.…”

“…d) Characteristic stage of charged practical pouch cells under lateral heating test. Reproduced with permission [78]. Copyright 2022, Wiley.…”

Scanning Electrochemical Microscopy Featuring Transient Current Signals in Carbon Nanopipets with Dilute or No Redox Mediator

“…Scanning electrochemical microscopy (SECM) and scanning ion conductance microscopy (SICM) are powerful in situ noninvasive techniques to acquire the local topography and activity imaging , of the substrates by monitoring the electron transfer or ion transport current signals, , and thus find broad applications in various emerging fields , including electrocatalysis, , single cell analysis, , corrosion, and sensing . Recently, the development of nanoelectrodes further put forward a higher desire for nanoscale SECM/SICM techniques with high temporal and spatial resolutions , toward revealing the local structure–activity relationship at the catalysis surface, ,− uncovering the dynamics of single molecules, − and realizing the imaging and analysis of single living cells. , …”