Composite Ionogel Electrodes for Polymeric Solid-State Li-Ion Batteries.

Realizing rechargeable cells with practical energy and power density requires electrodes with high active material loading, a remaining challenge for solid-state batteries. Here, we present a new strategy based on ionogel-derived solid-state electrolytes (SSEs) to form composite electrodes that enable high active material loading (>10 mg/cm2, ~9 mA/cm2 at 1C) in a scalable approach for fabricating Li-ion cells. By tuning the precursor and active materials composition incorporated into the composite lithium titanate electrodes, we achieve near-theoretical capacity utilization at C/5 rates and cells capable of stable cycling at 5.85 mA/cm2 (11.70 A/g) with over 99% average Coulombic efficiency at room temperature. Finally, we demonstrate a complete polymeric solid-state cell with a composite anode and a composite lithium iron phosphate cathode with ionogel SSEs, which is capable of stable cycling at a 1C rate.

Tunable Intervalence Charge Transfer in Ruthenium Prussian Blue Analog Enables Stable and Efficient Biocompatible Artificial Synapses.

Emerging concepts for neuromorphic computing, bioelectronics, and brain-computer interfacing inspire new research avenues aimed at understanding the relationship between oxidation state and conductivity in unexplored materials. This report expands the materials playground for neuromorphic devices to include a mixed valence inorganic 3D coordination framework, a ruthenium Prussian blue analog (RuPBA), for flexible and biocompatible artificial synapses that reversibly switch conductance by more than four orders of magnitude based on electrochemically tunable oxidation state. The electrochemically tunable degree of mixed valency and electronic coupling between N-coordinated Ru sites controls the carrier concentration and mobility, as supported by density functional theory computations and application of electron transfer theory to in situ spectroscopy of intervalence charge transfer. Retention of programmed states is improved by nearly two orders of magnitude compared to extensively studied organic polymers, thus reducing the frequency, complexity, and energy costs associated with error correction schemes. This report demonstrates dopamine-mediated plasticity of RuPBA synapses and biocompatibility of RuPBA with neuronal cells, evoking prospective application for brain-computer interfacing.

Room-Temperature Pseudo-Solid-State Iron Fluoride Conversion Battery with High Ionic Conductivity.

Li-metal batteries (LMBs) employing conversion cathode materials (e.g., FeF3) are a promising way to prepare inexpensive, environmentally friendly batteries with high energy density. Pseudo-solid-state ionogel separators harness the energy density and safety advantages of solid-state LMBs, while alleviating key drawbacks (e.g., poor ionic conductivity and high interfacial resistance). In this work, a pseudo-solid-state conversion battery (Li-FeF3) is presented that achieves stable, high rate (1.0 mA cm-2) cycling at room temperature. The batteries described herein contain gel-infiltrated FeF3 cathodes prepared by exchanging the ionic liquid in a polymer ionogel with a localized high-concentration electrolyte (LHCE). The LHCE gel merges the benefits of a flexible separator (e.g., adaptation to conversion-related volume changes) with the excellent chemical stability and high ionic conductivity (∼2 mS cm-1 at 25 °C) of an LHCE. The latter property is in contrast to previous solid-state iron fluoride batteries, where poor ionic conductivities necessitated elevated temperatures to realize practical power levels. The stable, room-temperature Li-FeF3 cycling performance obtained with the LHCE gel at high current densities paves the way for exploring a range of architectures including flexible, three-dimensional, and custom shape batteries.