Batteries are the most abundant form of electrochemical energy storage. Lithium and sodium ion batteries account for a significant portion of the battery market, but high-performance electrochemically active materials still need to be discovered and optimized for these technologies. Recently, tin(II) oxide (SnO) has emerged as a highly promising battery electrode. In this work, we present a facile synthesis method to produce SnO microparticles whose size and shape can be tailored by changing the solvent nature. We study the complex relationship between wet-chemistry synthesis conditions and resulting layered nanoparticle morphology. Furthermore, high-level electronic structure theory, including dispersion corrections to account for van der Waals forces, is employed to enhance our understanding of the underlying chemical mechanisms. The electronic vacuum alignment and surface energies are determined, allowing the prediction of the thermodynamically favoured crystal shape (Wulff construction) and surface-weighted work function. Finally, the synthesized nanomaterials were tested as Li-ion battery anodes, demonstrating significantly enhanced electrochemical performance for morphologies obtained from specific synthesis conditions.

Additive manufacturing strategies are gaining more importance in the context of lithium‐ion batteries. The rapid prototyping, reduced waste and complex 3D structures achievable are powerful and attractive tools that are out of the reach of current fabrication techniques. Additionally, thanks to the potential that these manufacturing techniques hold for the fabrication of micro‐energy storage devices, they are gaining increasing attention in the literature. Here, some of the more common additive manufacturing techniques are compared to standard methodologies by systematically evaluating their electrochemical performance and correlating it with the physical changes induced by the printing process. By using LTO/CNT‐based inks, it is observed that the inner arrangement of the conductive additive is significatively altered depending on the technique used and that this has an impact on the rate performance of the device. By using a model that links the capacity‐rate data to the physical properties of the batteries, it is possible to find the limiting factor on the printed electrodes and correlate it with the material arrangement that each technique produces.

One of the weaknesses of silicon-based batteries is the rapid deterioration of the charge-storage capacity with increasing cycle numbers. Pure silicon anodes tend to suffer from poor cycling ability due to the pulverization of the crystal structure after repeated charge and discharge cycles. In this work, we present the synthesis of a hollow nanostructured SiO 2 material for lithium-ion anode applications to counter this drawback. To improve the understanding of the synthesis route, the crucial synthesis step of removing the ZnO template core is shown using an in situ closed gas-cell sample holder for transmission electron microscopy. A direct visual observation of the removal of the ZnO template from the SiO 2 shell is yet to be reported in the literature and is a critical step in understanding the mechanism by which these hollow nanostructures form from their core−shell precursors for future electrode material design. Using this unique technique, observation of dynamic phenomena at the individual particle scale is possible with simultaneous heating in a reactive gas environment. The electrochemical benefits of the hollow morphology are demonstrated with exceptional cycling performance, with capacity increasing with subsequent charge−discharge cycles. This demonstrates the criticality of nanostructured battery materials for the development of next-generation Li + -ion batteries.