title: Tracking areal lithium densities from neutron activation - quantitative Li determination in self-organized TiO2nanotube anode materials for Li-ion batteries.
abstract: Nanostructuring of electrode materials is a promising approach to enhance the performance of next-generation, high-energy density lithium (Li)-ion batteries. Various experimental and theoretical approaches allow for a detailed understanding of solid-state or surface-controlled reactions that occur in nanoscaled electrode materials. While most techniques which are suitable for nanomaterial investigations are restricted to analysis widths of the order of Å to some nm, they do not allow for characterization over the length scales of interest for electrode design, which is typically in the order of mm. In this work, three different self-organized anodic titania nanotube arrays, comprising as-grown amorphous titania nanotubes, carburized anatase titania nanotubes, and silicon coated carburized anatase titania nanotubes, have been synthesized and studied as model composite anodes for use in Li-ion batteries. Their 2D areal Li densities have been successfully reconstructed with a sub-millimeter spatial resolution over lateral electrode dimensions of 20 mm exploiting the6Li(n,α)3H reaction, in spite of the extremely small areal Li densities (10-20 μg cm-2Li) in the nanotubular active material. While the average areal Li densities recorded via triton analysis are found to be in good agreement with the electrochemically measured charges during lithiation, triton analysis revealed, for certain nanotube arrays, areas with a significantly higher Li content ('hot spots') compared to the average. In summary, the presented technique is shown to be extremely well suited for analysis of the lithiation behavior of nanostructured electrode materials with very low Li concentrations. Furthermore, identification of lithiation anomalies is easily possible, which allows for fundamental studies and thus for further advancement of nanostructured Li-ion battery electrodes.
authors.affiliation: Leopold-Franzens-University Innsbruck, Institute of Physical Chemistry, Innrain 52c, Innsbruck, 6020, Austria. Engelbert.Portenkirchner@uibk.ac.at Julia.Kunze@uibk.ac.at.
authors.forename: E
authors.initials: E
authors.lastname: Portenkirchner
authors.forename: G
authors.initials: G
authors.lastname: Neri
authors.forename: J
authors.initials: J
authors.lastname: Lichtinger
authors.forename: J
authors.initials: J
authors.lastname: Brumbarov
authors.forename: C
authors.initials: C
authors.lastname: Rüdiger
authors.forename: R
authors.initials: R
authors.lastname: Gernhäuser
authors.forename: J
authors.initials: J
authors.lastname: Kunze-Liebhäuser