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Electrode processing plays an important role in advancing lithium-ion battery technologies and has a significant impact on cell energy density, manufacturing cost, and throughput. Compared to the extensive research on materials development, however, there has been much less effort in this area. In this Review, we outline each step in the electrode processing of lithium-ion batteries from materials to cell assembly, summarize the recent progress in individual steps, deconvolute the interplays between those steps, discuss the underlying constraints, and share some prospective technologies. This Review aims to provide an overview of the whole process in lithium-ion battery fabrication from powder to cell formation and bridge the gap between academic development and industrial manufacturing.

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High-voltage layered lithium- and manganese-rich (LMR) oxides have the potential to dramatically enhance the energy density of current Li-ion energy storage systems. However, these materials are currently not used commonly; one reason is their inability to maintain a consistent voltage profile (voltage fade) during electrochemical cycling. This report rationalizes the cause of this voltage fade by providing evidence of layered to spinel (LS) structural evolution pathways in the host Li1.2Mn0.55Ni0.15Co0.1O2 oxide. By employing neutron powder diffraction, we show that LS structural rearrangement in the LMR oxide occurs through a tetrahedral cation intermediate via the following: (i) diffusion of lithium atoms from octahedral to tetrahedral sites of the lithium layer [(LiLioct → LiLitet] which is followed by the dispersal of the lithium ions from the adjacent octahedral site of the metal layer to the tetrahedral sites of lithium layer [LiTMoct → LiLitet]; (ii) migration of Mn from the octahedral sites of the transition-metal layer to the “permanent” octahedral site of lithium layer via tetrahedral site of lithium layer [MnTMoct → MnLitet → MnLioct)]. These findings open the door to potential routes to mitigate this “atomic restructuring” in the high-voltage LMR composite oxide by manipulating their composition/structure for practical use in high-energy-density lithium-ion batteries.

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