The ability to 3D print lithium ion batteries (LIBs) in an arbitrary geometry would not only allow the battery form factor to be customized to fit a given product design but also facilitate the use of the battery as a structural component. A major hurdle to achieving this goal is the low ionic conductivity of the polymers used for 3D printing. This article reports the development of anode, cathode, and separator materials that enable 3D printing of complete lithium ion batteries with low cost and widely available fused filament fabrication (FFF) 3D printers. Poly(lactic acid) (PLA) was infused with a mixture of ethyl methyl carbonate, propylene carbonate, and LiClO 4 to obtain an ionic conductivity of 0.085 mS cm −1 , a value comparable to that of polymer and hybrid electrolytes. Different electrically conductive (Super P, graphene, multiwall carbon nanotubes) and active (lithium titanate, lithium manganese oxide) materials were blended into PLA to determine the relationships among filler loading, conductivity, charge storage capacity, and printability. Up to 30 vol % of solids could be mixed into PLA without degrading its printability, and an 80:20 ratio of conductive to active material maximized the charge storage capacity. The highest capacity was obtained with lithium titanate and graphene nanoplatelets in the anode, and lithium manganese oxide and multiwall carbon nanotubes in the cathode. We demonstrate the use of these novel materials in a fully 3D printed coin cell, as well as 3D printed wearable electronic devices with integrated batteries.
Materials that retain a high conductivity under strain are essential for wearable electronics. This article describes a conductive, stretchable composite consisting of a Cu-Ag core-shell nanowire felt infiltrated with a silicone elastomer. This composite exhibits a retention of conductivity under strain that is superior to any composite with a conductivity greater than 1000 S cm. This work also shows how the mechanical properties, conductivity, and deformation mechanism of the composite changes as a function of the stiffness of the silicone matrix. The retention of conductivity under strain was found to decrease as the Young's modulus of the matrix increased. This was attributed to void formation as a result of debonding between the nanowire felt and the elastomer. The nanowire composite was also patterned to create serpentine circuits with a stretchability of 300%.
This article reports a synthesis that yields 4.4 g of Cu nanowires in 1 h, and a method to coat 22 g of Cu nanowires with Ag within 1 h. Due to the large diameters of Cu nanowires (≈240 nm) produced by this synthesis, a Ag:Cu mol ratio of 0.04 is sufficient to coat the nanowires with ≈3 nm of Ag, and thereby protect them from oxidation. This multigram Cu‐Ag core–shell nanowire production process enabled the production of the first nanowire‐based conductive polymer composite filament for 3D printing. The 3D printing filament has a resistivity of 0.002 Ω cm, >100 times more conductive than commercially available graphene‐based 3D printing filaments. The conductivity of composites containing 5 vol% of 50‐µm‐long Cu‐Ag nanowires is greater than composites containing 22 vol% of 20‐µm‐long Ag nanowires or 10‐µm‐long flakes, indicating that high‐aspect ratio Cu‐Ag nanowires enable the production of highly conductive composites at relatively low volume fractions. The highly conductive filament can support current densities between 2.5 and 4.5 × 105 A m−2 depending on the surface‐to‐volume ratio of the printed trace, and was used to 3D print a conductive coil for wireless power transfer.
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