Formation and impact of nanoscopic oriented phase domains in electrochemical crystalline electrodes.

Electrochemical phase transformation in ion-insertion crystalline electrodes is accompanied by compositional and structural changes, including the microstructural development of oriented phase domains. Previous studies have identified prevailingly transformation heterogeneities associated with diffusion- or reaction-limited mechanisms. In comparison, transformation-induced domains and their microstructure resulting from the loss of symmetry elements remain unexplored, despite their general importance in alloys and ceramics.

A Nearly Packaging-Free Design Paradigm for Light, Powerful, and Energy-Dense Primary Microbatteries.

Billions of internet connected devices used for medicine, wearables, and robotics require microbattery power sources, but the conflicting scaling laws between electronics and energy storage have led to inadequate power sources that severely limit the performance of these physically small devices. Reported here is a new design paradigm for primary microbatteries that drastically improves energy and power density by eliminating the vast majority of the packaging and through the use of high-energy-density anode and cathode materials. These light (50-80 mg) and small (20-40 µL) microbatteries are enabled though the electroplating of 130 µm-thick 94% dense additive-free and crystallographically oriented LiCoO onto thin metal foils, which also act as the encapsulation layer.

Electrodeposition of atmosphere-sensitive ternary sodium transition metal oxide films for sodium-based electrochemical energy storage.

We introduce an intermediate-temperature (350 °C) dry molten sodium hydroxide-mediated binder-free electrodeposition process to grow the previously electrochemically inaccessible air- and moisture-sensitive layered sodium transition metal oxides, NaMO (M = Co, Mn, Ni, Fe), in both thin and thick film form, compounds which are conventionally synthesized in powder form by solid-state reactions at temperatures ≥700 °C. As a key motivation for this work, several of these oxides are of interest as cathode materials for emerging sodium-ion-based electrochemical energy storage systems. Despite the low synthesis temperature and short reaction times, our electrodeposited oxides retain the key structural and electrochemical performance observed in high-temperature bulk synthesized materials.

Revealing the role of the cathode-electrolyte interface on solid-state batteries.

Interfaces have crucial, but still poorly understood, roles in the performance of secondary solid-state batteries. Here, using crystallographically oriented and highly faceted thick cathodes, we directly assess the impact of cathode crystallography and morphology on the long-term performance of solid-state batteries. The controlled interface crystallography, area and microstructure of these cathodes enables an understanding of interface instabilities unknown (hidden) in conventional thin-film and composite solid-state electrodes.

Effects of Particle Size on Mg Ion Intercalation into λ-MnO Cathode Materials.

An emergent theme in mono- and multivalent ion batteries is to utilize nanoparticles (NPs) as electrode materials based on the phenomenological observations that their short ion diffusion length and large electrode-electrolyte interface can lead to improved ion insertion kinetics compared to their bulk counterparts. However, the understanding of how the NP size fundamentally relates to their electrochemical behaviors (e.g.