Restructuring the lithium-ion battery: A perspective on electrode architectures

The lithium-ion battery (LIB) has enabled portable energy storage, yet increasing societal demands have motivated a new generation of more advanced LIBs. Although the discovery and optimization of battery active materials has been the subject of extensive study since the 1980s, the most disruptive advancements of commercial LIBs in the past decade stem instead from overall cell design and engineering. In pursuit of higher energy density and fast-charging capability, strategies focused on tuning the properties of composite electrode architectures (e.g., porosity, conductivity, tortuosity, spatial heterogeneity) by restructuring the inactive component matrix of LIB electrode films have recently garnered attention. This perspective explores recent advances in electrode design through an applied lens, emphasizing synthetic platforms and future research directions that are scalable, commercially feasible, and applicable to a wide range of active materials. We introduce and critically assess recently proposed strategies for structuring electrode architectures, including spatial gradients of local composition and microstructure; metal-foil current collector alternatives; and electrode templating techniques, evaluating both achievements in battery performance and commercial applicability. Coupled with improved active materials, new electrode architectures hold promise to unlock next generation LIBs.