Publication date: 10th April 2024
Sulfide solid electrolytes have attracted considerable attention in the field of all-solid-state batteries due to their impressive ionic conductivity and ease of electrode integration. However, their inherent high reactivity predisposes them to undesirable interactions with cathodes, leading to the formation of detrimental interfacial layers that undermine the electrochemical performance of all-solid-state cells. This study departs from the conventional practice of costly surface coating using expensive precursors. Instead, it uses several oxides, namely Nb2O5, Ta2O5, and La2O3, as dopants in the precursor, an intermediate stage prior to cathode fabrication. This novel approach aims to enhance the stability of the cathode/sulfide electrolyte interface. The resulting doped cathodes showed remarkable improvements in both discharge capacity and rate capability. In addition, the introduction of doping resulted in significant improvements in cyclic performance and a significant reduction in impedance resistance. Considering the comprehensive analysis including SEM, TEM and XPS techniques, the distribution of the dopants within the cathode was not uniform but exhibited a gradient concentration profile with elevated levels at the surface. The doping, particularly evident in the case of Nb and Ta doping, was accompanied by a reduction in cation mixing due to subtle adjustments in the crystal structure and increased ionic conductivity. The results of XPS and high-resolution TEM studies also confirmed that gradient doping effectively limits unwanted side reactions with the cathode. This improvement is attributed to the formation of a coating-like protective layer formed at the interfacial region, coupled with the structural stabilization attributed to the doping process. These collective results validate the notion that the interfacial layer realized by gradient doping has a parallel protective capability as conventional surface coating.
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