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This dissertation deals with the electrode materials, liquid and gel electrolytes suitable for supercapacitors. In the field of electrode materials were investigated carbon materials based on carbon blacks, expanded and micronized graphite suitable for supercapacitors working on the principle electrochemical double layer. Another area which this thesis deals with are aprotic liquid electrolytes prepared from suitable types of salts and aprotic solvents. The last part is focused on the preparation and subsequent electrochemical characterization of gel polymer electrolytes in order to increase the ionic conductivity of these electrolytes.

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This paper deals with the construction of photoelectrochemical cell, used for detection of ultraviolet radiation as a UV sensor. Photoelectrochemical cell consists of three layers, layer of photoactive semiconductor titanium dioxide, carbon electrodes and poly(vinyl alcohol) polymer electrolyte. The sensor layer enables the detection of UV radiation with the subsequent generation of photocurrent. Material printing techniques, such as screenprinting, pad printing and inkjet printing were used to produce the cell. Gel electrolyte was characterized by optical microscopy and rheometry. Sensor functionality was verified by use of electroanalytical techniques.

The demand for electric vehicles is increasing rapidly as the world is preparing for a fossil fuel-free future in the automotive field. Lithium battery technologies are the most effective options to replace fossil fuels due to their higher energy densities. However, safety remains a major concern in using lithium as the anode, and the development of non-volatile, non-flammable, high conductivity electrolytes is of great importance. In this dissertation, a gel polymer electrolyte (GPE) consisting of ionic liquid, lithium salt, and a polymer has been developed for their application in lithium batteries. A comparative study between GPE and ionic liquid electrolyte (ILE) containing batteries shows a superior cyclic performance up to 5C rate and a better rate capability for 40 cycles for cells with GPE at room temperature. The improvement is attributed to GPE’s improved stability voltage window against lithium as well as higher lithium transference number. The performance of the GPE in lithium-sulfur battery system using sulfur-CNT cathodes shows superior rate capability for the GPE versus ILE for up to 1C rates. Also, GPE containing batteries had higher capacity retention versus ILE when cycled for 500 cycles vii at C/2 rate. Electrochemical impedance spectroscopy (EIS) studies reveal interfacial impedances for ILE containing batteries grew faster than in GPE batteries. The accumulation of insoluble Li2S2/Li2S on the electrodes decreases the active material thus contributes to capacity fading. SEM imaging of cycled cathodes reveals cracks on the surface of cathode recovered from ILE batteries. On the other hand, the improved electrochemical performance of GPE batteries indicates better and more stable passivation layer formation on the surface of the electrodes. Composite GPE (cGPE) containing micro glass fillers were studied to determine their electrochemical performance in Li batteries. GPE with 1 wt% micro fillers show superior rate capability for up to 7C and also cyclic stability for 300 cycles at C/2 rate. In situ, EIS also reveals a rapid increase in charge transfer resistance in GPE batteries, responsible for lowering the capacity during cycling. Improved ion transport properties due to ion-complex formations in the presence of the micro fillers, is evidenced by improved lithium transference number, ionic conduction, and ion-pair dissociation detected using Raman spectroscopy.

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Understanding molecular and ion dynamics in soft materials used for fuel cell, battery, and drug delivery vehicle applications on multiple time and length scales provides critical information for the development of next generation materials. In this dissertation, new insights into transport and kinetic processes such as diffusion coefficients, translational activation energies (Ea), and rate constants for molecular exchange, as well as how these processes depend on material chemistry and morphology are shown. This dissertation also aims to serve as a guide for material scientists wanting to expand their research capabilities via nuclear magnetic resonance (NMR) techniques. By employing variable temperature pulsed-field-gradient (PFG) NMR diffusometry, which can probe molecular transport over nm – μm length scales, I first explore transport and morphology on a series of ion-conducting materials: an organic ionic plastic crystal, a proton-exchange membrane, and a polymer-gel electrolyte. These studies show the dependencies of small molecule and ion transport on modulations to material parameters, including thermal or magnetic treatment, water content, and/or crosslink density. I discuss the fundamental significance of the length scale over which translational Ea reports on these systems (~ 1 nm) and the resulting implications for using the Arrhenius equation parameters to understand and rationally design new ion-conductors. Next, I describe how NMR spectroscopy can be utilized to investigate the effect of loading a small molecule into the core of a spherical block copolymer micelle (to mimic, e.g., drug loading) on the hydrodynamic radius (rH) and polymer chain dynamics. In particular, I present spin-lattice relaxation (T1) results that directly measure single chain exchange rate kexch between micelles and diffusion results that inform on the unimer exchange mechanism. These convenient NMR methods thus offer an economical alternative (or complement) to time-resolved small angle neutron scattering (TR-SANS). / Ph. D. / Lithium ion batteries, fuel cells, and drug-delivery vehicles each depend on a fundamental understanding of the interface between materials science and molecular dynamics. Optimization of such materials usually requires routine analysis through common polymer characterization techniques. The present dissertation highlights the usage of an uncommon analytical tool to the polymer science community, nuclear magnetic resonance (NMR); and how it gives unprecedented access in gauging material performance when subjected to judicious multiscale analysis. Chemical specificity, non-destructiveness, and the ability to study dynamics on multi-time and length scales are only a few of the many advantages of NMR offers over other polymer characterization techniques. Chapters 3, 4, 5, 6, and 7 investigate different classes of materials for their respective applications to better understand the aforementioned interface. These studies are intended to spark interest in new research areas while supplementing existing ones.