Self‐Assembly of 0D–2D Heterostructure Electrocatalyst from MOF and MXene for Boosted Lithium Polysulfide Conversion Reaction

Abstract The design of nanostructured electrocatalysts with high activity and long‐term durability for the sluggish lithium polysulfide (LiPS) conversion reaction is essential for the development of high‐performance lithium–sulfur (Li–S) batteries. Here, the self‐assembly of bimetallic selenides on nitrogen‐doped MXene (CoZn‐Se@N‐MX) based on the self‐assembly of metal–organic framework and MXene is reported. A combination of 0D CoZn‐Se nanoparticles and 2D N‐MX nanosheet co‐catalysts forms double lithiophilic‐sulfifilic binding sites that effectively immobilize and catalytically convert LiPS intermediates. This 0D–2D heterostructure catalyst has a hierarchical porous architecture with a large active area and enables rapid Li ion diffusion, reduces the activation energy of Li 2 S deposition, and lowers the energy barrier of Li 2 S dissolution. In addition, an assembled CoZn‐Se@N‐MX hybrid synergistically prevents the aggregation of the CoZn‐Se nanoparticles and restacking of the active areas of N‐MX nanosheets during assembly and the LiPS conversion process. The Li–S battery with this 0D–2D catalyst delivers excellent rate capability, ultralong cycling life (over 2000 cycles), and a high areal capacity of 6.6 mAh cm −2 with a low electrolyte/sulfur ratio of 5 µL mg −1 .