Towards an Enhanced Understanding of Charge Transport and Charge Transfer Processes in Rechargeable Batteries

Lithium-ion batteries are the state-of-the-art electrochemical energy storage technology for a wide range of devices, ranging from small portable electronics to (hybrid) electric vehicles and even large-scale stationary storage applications. Their tremendous success over the past few decades has triggered continuously increasing interest in this technology, including potential alternatives that may provide further advances in terms energy and/or power density, fast-charging capability, cost, sustainability, and also geo‑strategic considerations. While the search for new materials and components is still driven partly by trial and error, most breakthroughs have been made based on an in-depth understanding of their physicochemical and electrochemical properties, and how they behave in a relevant environment.

Herein, some of our recent advances in enhancing our understanding of existing and potential alternative active and inactive materials will be presented. These advances include an improved comprehension of the charge transport and transfer processes at the lithium-electrolyte interface and the frequently overlooked impact of the current collector on the reversibility of the lithium deposition process. Moreover, a new class of electrode active materials for lithium-ion batteries and beyond will be introduced, involving the atom-scale reduction of redox-active centers in insertion-type metal oxide host matrices. While some of these results are rather fundamental at this stage, others may contribute to the realization of advanced rechargeable batteries in the near to mid-term future.