The effect of extended H₂ sorption cycles on the structure and on the hydrogen storage performances of MgH₂ powders with 5 wt% of Fe particle catalyst is reported. MgH₂ powders with and without Fe have been ball milled under Argon, the doped MgH₂ nanocomposite has been cycled under hydrogen pressure up to a maximum of 47 desorption and absorption cycles at 300 °C. After acceleration during the first 10 cycles, the kinetics behavior of doped MgH₂ is constant after extended cycling, in terms of maximum storage capacity and rate of sorption. The major effect of cycling on particle morphology is the progressive extraction of Mg from the MgO shell surrounding the powder particles. The Mg extraction from the MgO shell leaves the catalyst particles inside the hydride particles. Many empty MgO shells are observed in the pure ball milled MgH₂ upon cycling at higher temperature, suggesting that this enhancement of the extraction efficiency is related to the higher operating temperature which favors Mg diffusivity with respect to the H ion one.

Activated hard carbons, obtained from the pyrolysis of various waste biomasses, were prepared and characterized for use as the active material for the fabrication of battery electrodes. The preparation consisted of a pyrolysis process, followed by an activation with KOH and a further high-temperature thermal process. TG and DTA were used to discriminate the steps of the activation process, while SEM, XRD, and Raman characterization were employed to evaluate the effects of activation. The activated carbons were tested as electrodes in lithium-sulfur and lithium-ion batteries. The carbonaceous materials coming from cherry stones and walnut shells have proved to be particularly suitable as electrode components. When used as anodes in lithium-ion batteries, both carbons exhibited a high first cycle discharge capacity, which was not restored during the next charge. After the first two cycles, in which there was a marked loss of capacity, both electrodes showed good reversibility. When used as cathodes in lithium-sulfur batteries, both carbons exhibited good catalytic activity against the redox reaction involving sulfur species with good cycle stability and satisfactory Coulombic efficiency.

Carbon nanostructures are highly promising materials for applications in a variety of different fields. Besides their interesting performances, the possibility to synthesize them from biowaste makes them an eco-friendly resource widely exploitable within a circular economy context. The present work deals with the green, one-pot synthesis of graphene quantum dots (GQDs) from carbon aerogels (CAs) derived from rice husk (RH). After having obtained CAs upon purification of RH, followed by gelification and carbonization of the resulting cellulose, the one-pot solventless production of GQDs was obtained by ball milling. This method determined the formation of crystalline nanostructures with a diameter of around 20 nm, which were analyzed via scanning electron microscopy, transmission electron microscopy, atomic force microscopy, X-ray diffraction, and Raman spectroscopy to obtain a full morphological and structural characterization. GQDs were used as electrode materials for supercapacitors and Li-ion batteries, showing the ability to both accumulate charges over the surface and intercalate lithium-ions. The reported results are a proof of principle of the possibility of exploiting GQDs as support material for the development of advanced systems for energy storage.

The advent of the lithium-ion batteries (LIBs) has transformed the energy storage field, leading to significant advances in electronics and electric vehicles, which continuously demand more and more performant devices. However, commercial LIB systems are still far from satisfying applications operating in arduous conditions, such as temperatures exceeding 100 °C. For instance, safety issues, materials degradation, and toxic stem development, related to volatile, flammable organic electrolytes, and thermally unstable salts (LiPF₆), limit the operative temperature of conventional lithium-ion batteries, which only occasionally can exceed 50–60 °C. To overcome this highly challenging drawback, the present study proposes advanced electrolyte technologies based on innovative, safer fluids such as ionic liquids (ILs). Among the IL families, we have selected ionic liquids based on tetrabutylphosphonium and 1-ethyl-3-methyl-imidazolium cations, coupled with per(fluoroalkylsulfonyl)imide anions, for standing out because of their remarkable thermal robustness. The thermal behaviour as well as the ion transport properties and electrochemical stability were investigated even in the presence of the lithium bis(trifluoromethylsulfonyl)imide salt. Conductivity measurements revealed very interesting ion transport properties already at 50 °C, with ion conduction values ranging from 10⁻³ and 10⁻² S cm⁻¹ levelled at 100 °C. Thermal robustness exceeding 150 °C was detected, in combination with anodic stability above 4.5 V at 100 °C. Preliminary cycling tests run on Li/LiFePO₄ cells at 100 °C revealed promising performance, i.e., more than 94% of the theoretical capacity was delivered at a current rate of 0.5C. The obtained results make these innovative electrolyte formulations very promising candidates for high-temperature LIB applications and advanced energy storage systems.

In this work, electrospun nanofiber membranes are investigated as separators for lithium batteries. Membrane consisting of polyacrylonitrile-polycaprolactone mixtures were produced following a combinatorial approach inspired by design of experiments to identify the relationships between process parameters and microstructural properties. The microstructure of the non-woven fibrous mats was characterized by scanning electron microscopy to measure thickness and fiber distribution. Temperature and relative humidity during membrane deposition were also tracked to include them in the statistical analysis and highlight their influence on the properties of the resulting membranes. The functional evaluation of the membranes was conducted by electrochemical impedance spectroscopy, after soaking the membrane in the electrolyte, to measure ion transport properties. All the separators showed specific conductivities higher than 1.5 × 10⁻³ S. The electrochemical performance was also evaluated when the membranes were used as actual separators in coin-cells assembled in-house, stacking the electrolyte-soaked membranes between a lithium anode and a LiFePO₄-based cathode. Among all, the PAN/PCL 50:50 showed excellent cycling stability, with a high initial capacity of 150 mAhg⁻¹ and a coulombic efficiency of 99.6%.