%0 Journal Article %T Sulfurized Two-Dimensional Conductive Metal-Organic Framework as a High-Performance Cathode Material for Rechargeable Mg Batteries. %A Mu Y %A Nyakuchena J %A Wang Y %A Wilkes JR %A Luo T %A Goldstein M %A Elander B %A Mohanty U %A Bao JL %A Huang J %A Wang D %J Angew Chem Int Ed Engl %V 0 %N 0 %D 2024 Jul 17 %M 39018503 %F 16.823 %R 10.1002/anie.202409286 %X Rechargeable Mg batteries are a promising energy storage technology to overcome the limitations inherent to Li ion batteries. A critical challenge in advancing Mg batteries is the lack of suitable cathode materials. In this work, we report a cathode design that incorporates S functionality into two-dimensional metal-organic-frameworks (2D-MOFs). This new cathode material enables good Mg2+ storage capacity and outstanding cyclability. It was found that upon the initial Mg2+ insertion and disinsertion, there is an apparent structural transformation that crumbles the layered 2D framework, leading to amorphization. The resulting material serves as the active material to host Mg2+ through reduction and/or oxidation of S and, to a limited extent, O. The reversible nature of S and O redox chemistry was confirmed by spectroscopic characterizations and validated by density functional calculations. Importantly, during the Mg2+ insertion and disinsertion process, the 2D nature of the framework was maintained, which plays a key role in enabling the high reversibility of the MOF cathode.