Nanoarchitecture factors of solid electrolyte interphase formation via 3D nano-rheology microscopy and surface force-distance spectroscopy

Abstract

The solid electrolyte interphase in rechargeable Li-ion batteries, its dynamics and, significantly, its nanoscale structure and composition, hold clues to high-performing and safe energy storage. Unfortunately, knowledge of solid electrolyte interphase formation is limited due to the lack of in situ nano-characterization tools for probing solid-liquid interfaces. Here, we link electrochemical atomic force microscopy, three-dimensional nano-rheology microscopy and surface force-distance spectroscopy, to study, in situ and operando, the dynamic formation of the solid electrolyte interphase starting from a few 0.1 nm thick electrical double layer to the full three-dimensional nanostructured solid electrolyte interphase on the typical graphite basal and edge planes in a Li-ion battery negative electrode. By probing the arrangement of solvent molecules and ions within the electric double layer and quantifying the three-dimensional mechanical property distribution of organic and inorganic components in the as-formed solid electrolyte interphase layer, we reveal the nanoarchitecture factors and atomistic picture of initial solid electrolyte interphase formation on graphite-based negative electrodes in strongly and weakly solvating electrolytes.

Voltage Hysteresis of Silicon Nanoparticles: Chemo‐Mechanical Particle‐SEI Model

“…The literature states values of Young's modulus of the SEI E SEI between only a few hundreds of MPa and values greater than 100 GPa. For a better overview, we divide the reported values into the categories: soft with E SEI < 1 GPa, [ 63–67 ] medium with 1 GPa ⩽ E SEI < 10 GPa, [ 63,66,68–72 ] stiff with 10 GPa ⩽ E SEI < 100 GPa, [ 53,68–70,73–75 ] and very stiff SEI with E SEI ⩾ 100 GPa. [ 68,75 ] In general, references report lower values of Young's modulus for thicker SEI layers.…”

“…Recently, research has advanced in estimating the viscosity value of the outer, organic SEI layer. [ 67,75 ] However, the inner, inorganic SEI layer is known to be much stiffer than the outer layer. We assume this coincides with a considerably higher viscosity of the inner layer.…”

Electrical Double Layer Formation at Intercalation Cathode–Organic Electrolyte Interfaces During Initial Lithium‐Ion Battery Reactions

“…Furthermore, the majority of experimental studies have been conducted on metal electrode-liquid electrolyte interfaces. [7,11] Thus, EDL research has been dominated by studies using computational methods such as molecular dynamics, [12] which could not give direct evidences regarding the interfacial structures.…”

Intramolecular Charge Transfer of Gold Nanoclusters for pH Indicating

“…Nanotechnology advancement has attracted much attention since nanoscale materials yield extraordinary physicochemical features, which can be precisely controlled down to atomic precision. , These properties can be utilized for fundamental research and potential applications in a variety of fields . Ultrasmall-sized metal nanoparticles with the core diameter less than 3 nm are referred to as nanoclusters (NCs). , Fluorescent NCs can be explored as excellent probes in biosensing, catalysis, bioimaging, and biomedicine. , They are key bridges between the atoms and nanoparticles.…”

“…1,2 These properties can be utilized for fundamental research and potential applications in a variety of fields. 3 Ultrasmall-sized metal nanoparticles with the core diameter less than 3 nm are referred to as nanoclusters (NCs). 4,5 Fluorescent NCs can be explored as excellent probes in biosensing, catalysis, bioimaging, and biomedicine.…”