High-Throughput Compositional and Structural Evaluation of a Li_a(Ni_xMn_yCo_z)O_r Thin Film Battery Materials Library

Abstract

A Lia(NixMnyCoz)Or cathode materials library was fabricated by combinatorial magnetron sputtering. The compositional analysis of the library was performed by a new high-throughput approach for Li-content measurement in thin films, which combines automated energy-dispersive X-ray spectroscopy, Deuteron-induced gamma emission, and Rutherford backscattering measurements. Furthermore, combining this approach with thickness measurements allows the mapping of density values of samples from the materials library. By correlating the obtained compositional data with structural data from high-throughput X-ray diffraction measurements, those compositions which show a layered (R3̅m) structure and are therefore most interesting for Li-battery applications (for cathode (positive) electrodes) can be rapidly identified. This structure was identified as being most pronounced in the compositions Li0.6(Ni0.16Mn0.35Co0.48)O2, Li0.7(Ni0.10Mn0.37Co0.51)O2, Li0.6(Ni0.23Mn0.33Co0.43)O2, Li0.3(Ni0.65Mn0.08Co0.26)O2, Li0.3(Ni0.63Mn0.08Co0.29)O2, Li0.4(Ni0.56Mn0.09Co0.34)O2, Li0.5(Ni0.45Mn0.13Co0.42)O2, and Li0.6(Ni0.34Mn0.14Co0.52)O2.

High‐Throughput Investigation of the Oxidation and Phase Constitution of Thin‐Film Ni–Al–Cr Materials Libraries

“…There were no indications for the occurrence of the phase Ni 5 Al 3 , which was reported for the bulk equilibrium phase diagram. [18] Compositional deviations of the phases Ni 2 Al 3 and Ni 3 Al of about 5 to 8 at% from their stoichiometric compositions are believed to be due the oxidation during which an oxide scale forms and binds a substantial amount of Al in this case.…”

High‐Throughput Experimentation and Computational Freeway Lanes for Accelerated Battery Electrolyte and Interface Development Research

“…To map (electro)chemical properties of the films, two main set up designs already exist to carry out measurements on a single planar substrate. These set ups are based either on a fixed array of cells generated on the top (the resolution is then limited by the intercell distance, measurements can be made simultaneously on several if not all cells), [ 165,166 ] or on an X – Y moving probe that can be positioned above each point of the substrate (the resolution is limited by the diameter of the tip from tens of µm (scanning electrochemical microscopy) to mm, the probe possibly contain a reference electrode, measurements have to be conducted sequentially). [ 167 ] The rest of the physical/chemical characterizations of the materials libraries is probably less straightforward given the thin film form of the materials, their possible amorphous character, and the presence of light elements (including Li).…”

“…To map (electro)chemical properties of the films, two main set up designs already exist to carry out measurements on a single planar substrate. These set ups are based either on a fixed array of cells generated on the top (the resolution is then limited by the intercell distance, measurements can be made simultaneously on several if not all cells), [165,166] or on an X-Y moving probe that can be positioned above each point of the substrate (the resolution is limited by the diameter of the tip from tens of µm (scanning electrochemical microscopy) to mm, the [136,144] Adapted with permission. [144] Copyright 2019, Springer Nature.…”

Discovery of new materials using combinatorial synthesis and high-throughput characterization of thin-film materials libraries combined with computational methods

“…By combining e.g., EDX with RBS and NRA, all elements in MLs of thin film Li-ion battery materials can be determined. 19 High-throughput X-ray diffraction (XRD) is used to determine the phases being present on a ML. XRD systems with microfocus source and area detector allow fast measurements with very good spatial resolution (spot size < 1 mm).…”