Foldable, High Energy Density Lithium Ion Batterie

Lithium Ion Batteries (LIBs) have become ubiquitous owing to its low cost, high energy density and, power density. Due to these advantages, LIBs have garnered a lot of attention as the primary energy storage devices in consumer electronics and electric vehicles. Recent advances in the consumer electronics research and, the drive to reduce greenhouse gases have created a demand for a shape conformable, high energy density batteries. This thesis focuses on the aforementioned two aspects of LIBs: (a) shape conformability (b) energy density and provides potential solutions to enhance them.;This thesis is divided into two parts viz. (i) achieving foldability in batteries and, (ii) improving its energy density. Conventional LIBs are not shape conformable due to two limitations viz. inelasticity of metallic foils, and delamination of the active materials while bending. In the first part of the thesis (in Chapter 3), this problem is solved by replacing metallic current collector with Carbon Nanotube Macrofilms (CNMs). CNMs are superelastic films comprising of porous interconnected nanotube network. Using Molecular Dynamics (MD) simulation, we found that in the presence of an interconnected nanotube network CNMs can be fully folded. This is because the resultant stress due to bending and, the effective bending angle at the interface is reduced due to the network of nanotubes. Hence, unlike an isolated nanotube (which ruptures beyond 120 degrees of bending), a network of nanotubes can be completely folded. Thus, by replacing metallic current collector foils with CNMs, the flexibility limitation of a conventional LIB can be transcended. The second part of this thesis focusses on enhancing the energy density of LIBs. Two strategies adopted to achieve this goal are (a) removing the dead weight of the batteries, and (b) incorporating high energy density electrode materials. By incorporating CNMs, the weight of the batteries was reduced by 5-10 times due to low mass loading of CNMs (0.7 mg/cm2) as compared to metallic foils (5-10 mg/cm2). We show that the energy density of the fully foldable battery with CMF current collectors can be up to 2-fold higher than conventional LIBs at realistic mass loading (5mg/cm2) of the electrode materials. Therefore, not only does the CMF impart shape conformability, it also significantly boosts the energy density of the device by removing the dead weight of the batteries.;Silicon (Si) shows enormous potential as the next generation anode material in Lithium-ion batteries due to its high energy denisty. However, Si is highly brittle, and in an effort to prevent Si from fracturing, the research community has migrated from the use of Si films to Si nanoparticle based electrodes. Such a strategy significantly reduces volumetric energy density due to the porosity of Si nanoparticle electrodes. In Chapters 4 and 5, we propose two solutions to incorporate Si films in foldable batteries. We show that contrary to conventional wisdom, Si films can be stabilized by two strategies: (a) anchoring the Si films to a carbon nanotube macrofilm (CNM) current-collector and (b) draping the films with a graphene monolayer. After electrochemical cycling, the graphene-coated Si films on CNM resembled a tough mud-cracked surface in which the graphene capping layer suppresses delamination and stabilizes the solid electrolyte interface by creating a slippery interface and reducing the stress transfer across the interface. The graphene-draped Si films on CNM exhibit long cycle life (> 1000 charge/discharge steps) with an average specific capacity of ~806 mAh/g. The volumetric capacity averaged over 1000 cycles of charge/discharge is ~2821 mAh/cm3 which is 2 to 5 times higher than what is reported in the literature for Si nanoparticle based electrodes. The graphene-draped Si anode could also be successfully cycled against commercial cathodes in a full-cell configuration. In Chapter 5, an alternate strategy has been explored to stabilize Si films by utilizing the role of a slippery interface in stabilizing Si. In this study, graphene films were used as a buffer layer on which Si films were deposited. Here, instead of a highly elastic matrix (as seen in Chapter 4), a slippery interface was used to stabilize Si. It was observed that due to the slippery interface, the Si films were stable and could retain a capacity of ~900 mAh/g. These Si films also possessed a volumetric capacity of ~5462 mAh/cm3. On the other hand, Si films with a rigid interface were completely eviscerated with a capacity retention of only 180 mAh/g.;Thus, this thesis presents new ideas to achieve foldable high energy density Lithium Ion Battery. We also hope that this thesis serves as a platform for researchers to further explore this field.