Construction of an Ohmic Contact Cathode by Two Metal Sulfides for efficient Capture and Catalysis of Polysulfide

Abstract The slow reaction kinetics and severe shuttle effect of lithium polysulfide make Li‐S battery electrochemical performance difficult to meet the demands of large electronic devices such as electric vehicles. Based on this, an electrocatalyst constructed by metal phase material (MoS 2 ) and semiconductor phase material (SnS 2 ) with ohmic contact is designed for inhibiting the dissolution of lithium polysulfide with improving the reaction kinetics. According to the density‐functional theory calculations, it is found that the heterostructured samples with ohmic contacts can effectively reduce the reaction‐free energy of lithium polysulfide to accelerate the sulfur redox reaction, in addition to the excellent electron conduction to reduce the overall activation energy. The metallic sulfide can add more sulfophilic sites to promote the capture of polysulfide. Thanks to the ohmic contact design, the carbon nanotube‐MoS 2 ‐SnS 2 achieved a specific capacity of 1437.2 mAh g −1 at 0.1 C current density and 805.5 mAh g −1 after 500 cycles at 1 C current density and is also tested as a pouch cell, which proves to be valuable for practical applications. This work provides a new idea for designing an advanced and efficient polysulfide catalyst based on ohmic contact.