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Spinel Li4Ti5O12 (LTO) is a promising anode material for solid state thin film batteries (SSTB) due to its almost-zero volume change and promising Li-ion mobility. However, preparing LTO anodes for SSTB demands tedious vacuum-based processing steps that are not cost effective. In this context, the present study embarks on evaluating the versatile suspension plasma spraying (SPS) approach to fabricate LTO coatings without using any binder. The microstructure and stoichiometry of the fabricated LTO coatings developed through the SPS route reveals retention of ∼76 wt.% of the spinel LTO from the starting feedstock, with minor amounts of rutile and anatase TiO2. The SPS experiments yielded varying thickness build up rates of the LTO coatings depending on the processing parameters adopted. The electrochemical data of the produced LTO based electrode tested in a half-cell through galvanostatic cycling show reversible lithiation and delithiation at expected potential, thereby validating the promise of the SPS technique for potential fabrication of SSTB components once fully optimized.

Alloy electrodes are attracting a lot of interest in the field of Li-ion batteries due to their high energy density. However, they suffer from large volume expansion and contraction during lithiation and delithiation, leading to rapid pulverization and disconnection. A strategy to avoid this is to use self-healing materials. Ga-based liquid alloys have been studied as self-healing electrodes because of their capacity to store Li and their liquid state at room temperature. The so-called "galinstan" (Ga0.77In0.15Sn0.08) exhibits the lowest melting temperatures and has also been used to add self-healing properties in composite electrodes. Nevertheless, its lithiation mechanism and its practical capacity still remain unknown. Also, the reversibility of the lithiation, which is crucial to ensure the self-healing properties offered by the liquid metal, requires investigation. In this work, electrochemical measurements were coupled with XRD and SEM analyses to better understand the redox processes, structural and morphological properties of galinstan as an electrode material in Li-ion batteries. It was shown that only Ga and In would react with Li to form LiGa and LiIn. The reversibility of these reactions and thus the self-healing ability of galinstan was demonstrated through observation of its liquid state before and after electrochemical cycling.

This study demonstrates the electrochemical sodiation and desodiation of gallium (Ga). A variety of techniques including galvanostatic cycling, cyclic voltammetry, as well as ex situ and in situ powder X-ray diffraction were used to determine the electrochemical reaction mechanisms. The sodiation and desodiation of Ga occurs reversibly at 0.71 V vs Na+/Na and the sodiated product was determined to be NaGa4 with a theoretical capacity of 96 mAh g(-1) (567 mAh cm(-3)). In addition, an anomalous plateau was observed at 0.66 V vs Na+/Na during the sodiation, which was attributed to a slow diffusion of Na into Ga particles. It was also shown that Na22Ga39 was not formed even if it is one of the expected compounds from the Ga-Na phases diagram. However, new crystalline structures were observed and were attributed to metastable phases of NaGa4.

Many of the challenges faced in the development of lithium-ion batteries (LIBs) and next-generation technologies stem from the (electro)chemical interactions between the electrolyte and electrodes during operation. It is at the electrode-electrolyte interfaces where ageing mechanisms can originate through, for example, the build-up of electrolyte decomposition products or the dissolution of metal ions. In pursuit of understanding these processes, X-ray photoelectron spectroscopy (XPS) has become one of the most important and powerful techniques in a large collection of available tools. As a highly surface-sensitive technique, it is often thought to be the most relevant in characterising the interfacial reactions that occur inside modern rechargeable batteries. This review tells the story of how XPS is employed in day-to-day battery research, as well as highlighting some of the most recent innovative in situ and operando methodologies developed to probe battery materials in ever greater detail. A large focus is placed not only on LIBs, but also on next-generation materials and future technologies, including sodium- and potassium-ion, multivalent, and solid-state batteries. The capabilities, limitations and practical considerations of XPS, particularly in relation to the investigation of battery materials, are discussed, and expectations for its use and development in the future are assessed.