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

Abstract 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.