Silicon is a promising alternative to the conventional graphite anodes due to its high theoretical capacity and favorable lithiation potential for lithium-ion batteries (LIBs) with liquid as well as solid-state electrolytes. However, lithiation-induced extreme volume change causes severe mechanochemical deformation and continuous formation of solid-electrolyte interphase leads to cell failure. One of the strategies to mitigate this problem is alloying silicon with a suitable element that can alter the surface electrochemistry and/or lithiation pathways, and acts as mechanical buffer. Nonetheless, these benefits come with a compromise on the specific capacity, which strongly influences the mass loading of the electrodes, highlighting the need to deconvolute the intertwined influence of composition and mass loading when designing high performance electrodes. In this work, we systematically studied the influence of composition and mass loading in monolithic amorphous silicon and non-stoichiometric silicon nitride (SiN_x) electrodes on their electrochemical performance as LIB anodes. The incorporation of nitrogen in the electrode matrix clearly improves the electrochemical stability at the expense of reduced specific capacity, while higher mass loading accelerates capacity fading, most critically in amorphous silicon electrodes. Postmortem analysis reveals that such capacity fading in the electrodes with higher mass loading can be related to delamination due to evolved tensile stress during the charge–discharge cycle. Yet, nitrogen-rich SiN_x monolithic electrodes accommodate strain more effectively. These findings demonstrate that while pristine Si delivers high specific capacity and long-term stability in thin films, thicker (>1 µm) monolithic electrodes benefit from higher nitrogen content in SiN_x, which provides more stable cycling and sustained capacity. ... Read more

This study investigates the influence of reactive sputtering gas composition, specifically the oxygen-to-argon (O2/Ar) and hydrogen-to-argon (H2/Ar) ratios, on the optoelectrical and structural properties of fluorine-doped tin oxide (FTO) and undoped tin dioxide (SnO2) thin films deposited at room temperature (RT). Through systematic variation of O2 and H2 content in the sputtering atmosphere, gas-phase composition is correlated with key performance metrics, including optical transmittance, sheet resistance, carrier density, and mobility, both before and after postdeposition annealing (PDA) at 400 °C in a nitrogen atmosphere. An optimal O2/Ar ratio of 0.3–0.4% achieves the best optoelectrical trade-off in FTO, yielding a minimum sheet resistance (468 Ω/sq) and high mobility (13.7 cm2/(V s)). In SnO2 films, increasing oxygen improves optical transparency but reduces conductivity, while hydrogen incorporation at fixed 1% O2/Ar enhances transparency and lowers sheet resistance in the as deposited state. These effects are attributed to defect passivation rather than changes in oxidation state, as supported by X-ray photoelectron spectroscopy results. Ambipolar conduction observed in the as deposited films transitions to stable n-type behavior after PDA, highlighting the role of thermal treatment. Although RT sputtered SnO2-based films do not yet match the performance of high-temperature grown benchmarks, these findings demonstrate that careful tuning of the sputtering gas composition enables scalable, thermally compatible, and cost-effective fabrication of transparent conducting electrodes and transport layers in photovoltaic applications. ... Read more