Universal Intercalation/Alloying Hybrid Mechanism with ‐ICOHP Criterion in MAX Toward Steadily Ascending Lithium‐Ion Batteries

Abstract Profiting from the unique atomic laminated structure, metallic conductivity, and superior mechanical properties, transition metal carbides and nitrides named MAX phases have shown great potential as anodes in lithium‐ion batteries. However, the complexity of MAX configurations poses a challenge. To accelerate such application, a minus integrated crystal orbital Hamilton populations descriptor is innovatively proposed to rapidly evaluate the lithium storage potential of various MAX, along with density functional theory computations. It confirms that surface A‐element atoms bound to lithium ions have odds of escaping from MAX. Interestingly, the activated A‐element atoms enhance the reversible uptake of lithium ions by MAX anodes through an efficient alloying reaction. As an experimental verification, the charge compensation and Sn_xLi_y phase evolution of designed Zr₂SnC MAX with optimized structure is visualized via in situ synchrotron radiation XRD and XAFS technique, which further clarifies the theoretically expected intercalation/alloying hybrid storage mechanism. Notably, Zr₂SnC electrodes achieve remarkably 219.8% negative capacity attenuation over 3200 cycles at 1 A g⁻¹. In principle, this work provides a reference for the design and development of advanced MAX electrodes, which is essential to explore diversified applications of the MAX family in specific energy fields.