Unlocking Superior Conductivity in MOF Electrodes via a MXene‐Activated Electronic Inversion Layer

ABSTRACT Metal‐organic frameworks (MOFs) are rising stars for Li‐ion batteries (LIBs) electrodes. However, low conductivity of MOFs easily caused polarization and poor active site utilization. Here, an innovative electronic inversion layer (EIL) was proposed to guide the composite and interface design of MIL‐53(Fe) with Ti 3 C 2 T x , prompting a remarkable increase in the electrical conductivity of MIL‐53(Fe) from 4.94 × 10 −2 µS/cm to 46.65 mS/cm (30 MPa). This enhancement is attributed to the EIL activated by Ti 3 C 2 T x effectively shift the primary charge carriers from holes to high‐mobility electrons. Simultaneously, the localized EIL promoted the formation of a p–n junction and establishes a hole concentration gradient in MIL‐53(Fe)@Ti 3 C 2 T x , thereby accelerating lithium‐ion diffusion kinetics. Consequently, the MIL‐53(Fe)@Ti 3 C 2 T x delivered a superior capacity of 450.3 mAh/g at 1 A/g, and the possible retention of 94% capacity after 1000 cycles, exceeding those of the MIL‐53(Fe) and Ti 3 C 2 T x . This investigation into MXene‐activated EIL presents an innovative strategy and mechanism of universal significance for addressing the inherent conductivity challenges acted by a series of electrode materials, especially MOFs and COFs.