High‐Throughput Screening of 1D Chalcogenide Cathode Materials Beyond VS4 for Rechargeable Magnesium‐ion Batteries

Owing to their high theoretical specific capacity and abundance of anodes, rechargeable Mg‐ion batteries (rMIBs) have emerged as a supplement for post‐Li generation. However, the strong Coulomb interactions on Mg2+ cations lead to inefficient storage and transport in the cathode, which severely restricts the actual performance of rMIBs. Herein, a virtual screening of the 1D material database (C1DB) is proposed to identify novel rMIB chalcogenide cathodes with large voids for relieving the Coulomb forces. By referring to the representative VS4 material, three potential 1D chalcogenide materials (SiS2, GeS2, and SiSe2) with optimized Coulomb interactions are ultimately screened out for rMIB cathodes. In addition, further theoretical analyses on geometry, electronic structures, and atomic charges reveal the significant roles of the large specific pore volume, low bond covalency, and mildly oxidizing anion element in optimizing rMIB cathode materials. Overall, our work may inspire future experimental and theoretical investigations, potentially accelerating breakthroughs of rMIB and other similar metal‐ion batteries.