A FIB-SEM Based Correlative Methodology for X-Ray Nanotomography and Secondary Ion Mass Spectrometry: An Application Example in Lithium Batteries Research

Abstract

Correlative microscopy approaches are attracting considerable interest in several research fields such as materials and battery research. Recent developments regarding X-ray computer tomography have made this technique available in a compact module for scanning electron microscopes (SEMs). Nano-computed tomography (nanoCT) allows morphological analysis of samples in a nondestructive way and to generate 2D and 3D overviews. However, morphological analysis alone is not sufficient for advanced studies, and to draw conclusions beyond morphology, chemical analysis is needed. While conventional SEM-based chemical analysis techniques such as energy-dispersive X-ray spectroscopy (EDS) are adequate in many cases, they are not well suited for the analysis of trace elements and low-Z elements such as hydrogen or lithium. Furthermore, the large information depth in typical SEM-EDS imaging conditions limits the lateral resolution to micrometer length scales. In contrast, secondary ion mass spectrometry (SIMS) can perform elemental mapping with good surface sensitivity, nanoscale lateral resolution, and the possibility to analyze even low-Z elements and isotopes. In this study, we demonstrate the feasibility and compatibility of a novel FIB-SEM-based correlative nanoCT-SIMS imaging approach to correlate morphological and chemical data of the exact same sample volume, using a cathode material of a commercial lithium battery as an example.

Learning-Based Approaches for Reconstructions With Inexact Operators in nanoCT Applications

“…One phantom has a main shape and up to 3 subshapes within (see Fig. 2), which is inspired by common experimental settings in nanoCT [17], [44], [45].…”

Toward Operando Structural, Chemical, and Electrochemical Analyses of Solid-State Batteries Using Correlative Secondary Ion Mass Spectrometry Imaging

“…The FIB-SEM instrument is equipped with an in-house-designed magnetic sector SIMS, and details about the FIB-SEM-SIMS instrument and its performance can be found elsewhere . The implementation of SIMS in the present operando study presents a huge advantage in terms of chemical analysis, allowing to detect and measure the distribution of low-Z elements such as H and Li. , Li often plays an important role in degradation mechanisms due to its high ionic mobility and capability to form dendrites, − and therefore, it is essential to observe the evolution of the Li distribution.…”

Thermal Recovery of the Electrochemically Degraded LiCoO2/Li7La3Zr2O12:Al,Ta Interface in an All-Solid-State Lithium Battery

“…We tracked the electrochemical degradation during cycling and demonstrated the recovery of the cells by a simple heating procedure. Advanced methods of interface analysis such as transmission electron microscopy (TEM), secondary ion mass spectrometry (SIMS), 38 and micro-Raman spectroscopy have been employed to gain insights into the macroscopic to the atomic scale. Finally, the experimental observations were validated by thermodynamic-based simulations using density functional theory (DFT).…”