Transparent, elastic conductors are essential components of electronic and optoelectronic devices that facilitate human interaction and biofeedback, such as interactive electronics, implantable medical devices and robotic systems with human-like sensing capabilities. The availability of conducting thin films with these properties could lead to the development of skin-like sensors that stretch reversibly, sense pressure (not just touch), bend into hairpin turns, integrate with collapsible, stretchable and mechanically robust displays and solar cells, and also wrap around non-planar and biological surfaces such as skin and organs, without wrinkling. We report transparent, conducting spray-deposited films of single-walled carbon nanotubes that can be rendered stretchable by applying strain along each axis, and then releasing this strain. This process produces spring-like structures in the nanotubes that accommodate strains of up to 150% and demonstrate conductivities as high as 2,200 S cm(-1) in the stretched state. We also use the nanotube films as electrodes in arrays of transparent, stretchable capacitors, which behave as pressure and strain sensors.
All-solid-state batteries promise significant safety and energy density advantages over liquid-electrolyte batteries. The interface between the cathode and the solid electrolyte is an important contributor to charge transfer resistance. Strong bonding of solid oxide electrolytes and cathodes requires sintering at elevated temperatures. Knowledge of the temperature dependence of the composition and charge transfer properties of this interface is important for determining the ideal sintering conditions. To understand the interfacial decomposition processes and their onset temperatures, model systems of LiCoO2 (LCO) thin films deposited on cubic Al-doped Li7La3Zr2O12 (LLZO) pellets were studied as a function of temperature using interface-sensitive techniques. X-ray photoelectron spectroscopy (XPS), secondary ion mass spectroscopy (SIMS), and energy-dispersive X-ray spectroscopy (EDS) data indicated significant cation interdiffusion and structural changes starting at temperatures as low as 300⁰C. La2Zr2O7 and Li2CO3 were identified as 2 decomposition products after annealing at 500°C by synchrotron X-ray diffraction (XRD). X-ray absorption spectroscopy (XAS) results indicate the presence of also LaCoO3, in addition to La2Zr2O7 and Li2CO3. Based on electrochemical impedance spectroscopy, and depth profiling of the Li distribution upon potentiostatic hold experiments on symmetric LCO|LLZO|LCO cells, the interfaces exhibited significantly increased impedance, up to 8 times that of the as-deposited samples after annealing at 500 o C. Our results indicate that lower-temperature processing conditions, shorter annealing time scales, and CO2-free environments are desirable for obtaining ceramic cathode-electrolyte interfaces that enable fast Li transfer and high capacity.
Flexible transparent electrodes are crucial for touch screen, flat panel display, and solar cell technologies. While carbon nanotube network electrodes show promise, characteristically poor dispersion properties have limited their practicality. We report that addition of small amounts of conjugated polymer to nanotube dispersions enables straightforward fabrication of uniform network electrodes by spin-coating and simultaneous tuning of parameters such as bundle size and density. After treatment in thionyl chloride, electrodes have sheet resistances competitive with other reported carbon nanotube based transparent electrodes to date.
MoO(x) has been used for organic semiconductor doping, but it had been considered an inefficient and/or unstable dopant. We report that MoO(x) can strongly and stably dope carbon nanotubes and graphene. Thermally annealed MoO(x)-CNT composites can form durable thin film electrodes with sheet resistances of 100 Ω/sq at 85% transmittance plain and 85 Ω/sq at 83% transmittance with a PEDOT:PSS adlayer. Sheet resistances change less than 10% over 20 days in ambient and less than 2% with overnight heating to 300 °C in air. The MoO(x) can be easily deposited either by thermal evaporation or from solution-based precursors. Excellent stability coupled with high conductivity makes MoO(x)-CNT composites extremely attractive candidates for practical transparent electrodes.
Complex chemomechanical interplay exists over a wide range of length scales within the hierarchically structured lithium-ion battery. At the mesoscale, the interdependent structural complexity and chemical heterogeneity collectively govern the local chemistry and, as a result, critically influence the cell level performance. Here we investigate the morphology and state of charge (SOC) inhomogeneity within secondary NCA particles that were cycled in solid polymer batteries. We observe substantial inhomogeneity in the nickel oxidation state (a proxy for SOC) and loss of structural integrity within secondary particles after only 20 cycles due to significant intergranular cracking. The formation of mesoscale cracks causes loss of ionic and electrical contact within cathode particles, triggering increases in local impedance and rearrangement of transport pathways for charge carriers. This can eventually lead to deactivation of sub-particle level domains in solid-state lithium-ion batteries. Our findings highlight the importance of proper mesoscale strain and defect management in polymer lithium-ion batteries.
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