Atomic-Scale Tailoring of Ni-Rich Cathodes for the Development of Commercial Li-Ion Batteries: From Laboratory to...

The rapid growth of the Li-ion battery industry has promoted the development of breakthrough materials and systems; nevertheless, achieving desired performance through sophisticated designs within well-established systems has also become essential. Here, it is demonstrated that precise control of the lithium-to-transition-metal (Li/M) ratio serves as a commercially viable lever to tune the voltage profile of Ni-rich cathodes. This arises from the combined effects of Ni defect at Li sites (Ni_Li) and the Ni oxidation state, as confirmed by experimental validation and density functional theory (DFT) calculations. This fundamental understanding establishes design rules for tailoring voltage profiles to meet application-specific cut-off voltages, thereby achieving optimal performance. This study presents a systematic framework for developing commercial cells based on atomic-scale design principles, ensuring industrial applicability.