This dissertation work has established a strong foundation for the pursuit of several exciting research topics. First, given the complexity of the ink formulations and the difficulty encountered in sequentially printing each component without interlayer mixing, experimentation with novel 2D and 3D architectures could not be explored in the given time frame. Architecture is one crucial research front in the pursuit of stretchable devices, and has also been shown to impact capacity retention and cell cycle lifetime in batteries. As stressed throughout this dissertation, additive manufacturing technologies are anticipated to enable rapid prototyping and exploration of a broad array of novel battery architectures, which could not easily be explored by traditional battery fabrication methods. Therefore, the utilization of additive manufacturing would allow one to probe an array of battery architectures including serpentine, interdigitated, and crossed patterns (Figure 7.1A-D), which have varying degrees of intrinsic flexibility/stretchability.
Beyond the enhanced mechanical effects of such macroscale patterns, micropatterning of electrodes was recently shown to significantly increase capacity retention and cell cycle lifetime by improving electrolyte wetting. This phenomenon could be exploited using additive manufacturing by creating hierarchical structures within the battery electrodes that have architectures geared towards macroscale flexibility/stretchablity, and that are decorated with printed capillary microstructure for improved battery performance.
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Figure 7.1. Overview of battery architectures and printable batteries. (A-D) Potential printing patterns such as (A) sheet, (B) crossed, (C) interdigitated, and (D) serpentine, where blue represents the cathode, yellow represents the anode, and green represents an overlapped cathode and anode separated by a polymer separator. Schematic representation of (E) the process of using filamentary printing to print an overlapped serpentine structured battery and (F) a PDMS encapsulated (light blue) overlapped serpentine battery capable of reversible stretching.
A second topic of research should be the development of a flexible encapsulant that is impermeable to both moisture and air. For flexible application, the only current choice for an encapsulant is the aluminum-polymer pouch typically used in industry. They come in a variety of thicknesses, but even the thinnest pouch available is susceptible to significant crease memory. Moreover, once these cells are vacuum sealed to ensure tight contact between all the battery components, the overall rigidity prevents them from being bent or folded at all. One possible route to achieving a truly flexible encapsulant for Li- ion batteries could be to ALD coat the Surlyn material used in Chapter 2 with a thin layer of material to act as a moisture/air barrier.
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Finally, it was observed during the thermal studies presented in Chapter 6 that there was potential for even higher temperature performance than what was demonstrated. If performance at temperatures exceeding 150 °C could be shown, this work would be a first of its kind for rechargeable Li-ion batteries. Unfortunately, the coin cell architecture we implemented used polypropylene gaskets to ensure a hermetic seal, but they were not able to withstand temperatures beyond 130 °C for any extended period of time. In addition, there was indication of performance irregularity during electrochemical cycling if the voltage window was not appropriately adjusted at elevated temperature. There are several possible causes believed to be behind this issue: (1) crystal structure breakdown of the LiFePO4 electrode at elevated temperature, (2) degradation of the imidazolium IL,
(3) formation of LiF during the dehydrofluorination of the CPE-PI membrane, or (4) unstable solid-electrolyte interphase formation on the Li metal anode. It would be worthwhile to study these causes and to pinpoint any major issues. For instance, one could monitor the crystal structure of the electrode when cycled at elevated temperatures.
129 8 Appendix
Figure 8.1. Effect of CC on electrolyte infiltration. White arrows in the photograph of the bottom side indicate the edge of the electrolyte spot. Scale bars: 0.5 cm.
130
Figure 8.2. Photographs of the process of fabricating Surlyn-encapsulated flexible full-cells. a) LiFePO4/MWNT (left) and Li4Ti5O12/MWNT (right) electrodes and separator membrane (center)
(b) Wire leads thermally laminated between two pieces of 75 µm Surlyn. c) 75 µm Surlyn pouch thermally sealed on three edges containing the electrodes, separator, and wire leads. A needle cap is contained in the opposite side of the pouch. d) Pouch after thermally sealing the final edge after folding. An additional seal was placed at the nanotube electrode leads. e) Pouch after addition of 0.8 mL liquid electrolyte (punctured pouch at the needle cap). Bubbles were kneaded away from the battery and sealed (middle of the pouch). A final seal was done closer to the
131
battery to remove new bubbles after the first charge. f) Sealed flexible battery used for in situ mechanical testing after cutting away the excess Surlyn. g) Metal foil full-cell in a Surlyn pouch made using the same procedure shown in (a-f). Scale bars: 1.0 cm
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