In Situ Electrochemical Reconstruction of Terephthalate Metal–Organic Framework Nanosheets for High‐Efficiency Lithium‐Ion Storage

Abstract The use of metal–organic frameworks (MOFs) as electrode materials in electrochemical energy storage is still limited to two options, except for a few electrochemically stable MOFs that can be directly used as electrodes. Most of the MOFs often serve as templates for preparing inorganic electrodes. This study demonstrates that terephthalate MOF nanosheet electrodes represent an alternative category for effective electrochemical Li + storage through an in situ electrochemical reconstruction mechanism. Upon the initial lithiation/de‐lithiation cycles, the original MOF nanosheet assembly transitions to a distinctive plum pudding‐like structure with massive metal oxide nanocrystals embedded in a porous lithium terephthalate matrix, which can deliver a high capacity of 1582.4 mAh g −1 at a current density of 0.1 A g −1 and maintain a reversible capacity of 502.6 mAh g −1 at 2 A g −1 after 2000 cycles. This study offers a valuable reference for designing MOF electrodes and advancing the applications of MOF materials in electrochemistry.