Toward a Synergistic Optimization of Porous Electrode Formulation and Polysulfide Regulation in Lithium-Sulfur Batteries.

The use of functional materials is a popular strategy to mitigate the polysulfide-induced accelerated aging of lithium-sulfur (Li-S) batteries. However, deep insights into the role of electrode design and formulation are less elaborated in the available literature. Such information is not easy to unearth from the existing reports on account of the scattered nature of the data and the big dissimilarities among the reported materials, preparation protocols, and cycling conditions. In this study, model functional materials known for their affinity toward polysulfide species, are integrated into the porous sulfur electrodes at different quantities and with various spatial distributions. The electrodes are assembled in 240 lithium-sulfur cells and thoroughly analyzed for their short- and long-term electrochemical performance. Advanced data processing and visualization techniques enable the unraveling of the impact of porous electrodes' formulation and design on self-discharge, sulfur utilization, and capacity loss. The results highlight and quantify the sensitivity of the cell performance to the synergistic interactions of catalyst loading and its spatial positioning with respect to the sulfur particles and carbon-binder domain. The findings of this work pave the road for a holistic optimization of the advanced sulfur electrodes for durable Li-S batteries.

A limitation map of performance for porous electrodes in lithium-ion batteries.

Driven by expanding interest in battery storage solutions and the success story of lithium-ion batteries, the research for the discovery and optimization of new battery materials and concepts is at peak. The generation of experimental (dis)charge data using coin cells is fast and feasible and proves to be a favorite practice in the battery research labs. The quantitative interpretation of the data, however, is not trivial and decelerates the process of screening and optimization of electrode materials and recipes. Here, we introduce the concept of polarographic map and demonstrate how it can be leveraged to quantify the contribution of different non-equilibrium phenomena to the performance limitation and total polarization of a lithium-ion cell. We showcase the accuracy and diagnostic power of this approach by preparing and analyzing the electrochemical performance of 54 sets of LiNixMnyCo1-x-yO2 electrodes with different formulations and designs discharged in a range of 0.2C-5C.