In this work, we introduce a method based on impedance spectroscopy and the equations developed to evaluate, with a good degree of accuracy, the number density, mobility and diffusion coefficient of mobile ions. Nyquist plots of electrolytes based on poly(acrylonitrile) or PAN and methyl cellulose (MC) incorporated with lithium bis(oxalato)borate have been established from impedance measurements. Equivalent circuits based on a resistor and “leaky capacitor(s)” have been determined and the relevant impedance equations derived. The values of the parameters required in the equation are obtained from the Nyquist plots and the parameters that cannot be obtained from the respective plots have been obtained by trial and error in order to fit the Nyquist plots. The transport parameters are calculated using the developed equations and the results have been compared with those obtained from the broadband dielectric response (BDR) method. Finally, Fourier transform infrared (FTIR) spectroscopy has been used to verify the results obtained from the two approaches at room and elevated temperatures.

Electrochemical devices, especially energy storage, have been around for many decades. Liquid electrolytes (LEs), which are known for their volatility and flammability, are mostly used in the fabrication of the devices. Dye-sensitized solar cells (DSSCs) and quantum dot sensitized solar cells (QDSSCs) are also using electrochemical reaction to operate. Following the demand for green and safer energy sources to replace fossil energy, this has raised the research interest in solid-state electrochemical devices. Solid polymer electrolytes (SPEs) are among the candidates to replace the LEs. Hence, understanding the mechanism of ions’ transport in SPEs is crucial to achieve similar, if not better, performance to that of LEs. In this paper, the development of SPE from basic construction to electrolyte optimization, which includes polymer blending and adding various types of additives, such as plasticizers and fillers, is discussed.

A poly(vinyledene difluoride)–lithium bis(oxalato)borate solid polymer electrolyte prepared by a solvent casting method has been irradiated with different doses of gamma-rays. Differential scanning calorimetry reveals that the polymer electrolyte irradiated with 35 kGy of γ-rays is the most amorphous sample. This is also supported by the results obtained from X-ray diffraction. The Fourier transform infrared spectrum of each irradiated sample has been deconvoluted in the wavenumber region between 1830 and 1758 cm⁻¹ in order to predict the percentage of free and contact ions in the samples. The sample exposed to 35 kGy of γ-rays contains the highest percentage of free ions and the lowest amount of contact ions. This sample also exhibits the highest room temperature conductivity of 3.05 × 10⁻⁴ S cm⁻¹, which is 15% higher relative to the virgin sample. The number density of free ions is observed to have more control on the conductivity variation with the γ-radiation dose compared to ionic mobility. This study confirms that γ-irradiation can be a potential way to obtain highly conductive and mechanically stable polymer electrolytes.