Sulfur (S) is an attractive cathode material with advantages including high theoretical capacity and low cost. However, issues such as the lithium polysulfide shuttle effect and its insulating properties greatly limit the future applications of lithium‐sulfur (Li‐S) batteries. Here, a viscous aqueous ink with nanoscale S uniformly decorated on the polar, metallically conductive titanium carbide MXene nanosheets (S@Ti3C2Tx) is reported to address these issues. Importantly, it is observed that the conductive Ti3C2Tx mediator efficiently chemisorbs the soluble polysulfides and converts them into thiosulfate/sulfate. The in situ formed sulfate complex layer acts as a thick protective barrier, which significantly retards the shuttling of polysulfides upon cycling and improves the sulfur utilization. Consequently, the binder‐free, robust, highly electrically conductive composite film exhibits outstanding electrochemical performance, including high capacities (1244–1350 mAh g‐1), excellent rate handling, and impressive cycling stability (0.035–0.048% capacity loss per cycle), surpassing the best MXene‐S batteries known. The fabrication of a pouch cell based on the freestanding S@Ti3C2Tx film is also reported. The prototype device showcases high capacities and excellent mechanical flexibility. Considering the broad family of MXenes and their unique roles in immobilizing the polysulfides, various S@MXene composites can be similarly fabricated with promising Li+ storage capability and long lifetime performance.
Freestanding, robust electrodes with high capacity and long lifetime are of critical importance to the development of advanced lithium-sulfur (Li-S) batteries for next-generation electronics, whose potential applications are greatly limited by the lithium polysulfide (LiPS) shuttle effect. Solutions to this issue have mostly focused on the design of cathode hosts with a polar, sulfurphilic, conductive network, or the introduction of an extra layer to suppress LiPS shuttling, which either results in complex fabrication procedures or compromises the mechanical flexibility of the device. A robust Ti 3 C 2 T x /S conductive paper combining the excellent conductivity, mechanical strength, and unique chemisorption of LiPSs from MXene nanosheets is reported. Importantly, repeated cycling initiates the in situ formation of a thick sulfate complex layer on the MXene surface, which acts as a protective membrane, effectively suppressing the shuttling of LiPSs and improving the utilization of sulfur. Consequently, the Ti 3 C 2 T x /S paper exhibits a high capacity and an ultralow capacity decay rate of 0.014% after 1500 cycles, the lowest value reported for Li-S batteries to date. A robust prototype pouch cell and full cell of Ti 3 C 2 T x /S paper // lithium foil and prelithiated germanium are also demonstrated. The preliminary results show that Ti 3 C 2 T x /S paper holds great promise for future flexible and wearable electronics.
Herein, two new two-dimensional Nb 4 C 3 -based solid solutions (MXenes), (Nb 0.8 ,Ti 0.2 ) 4 C 3 T x and (Nb 0.8 ,Zr 0.2 ) 4 C 3 T x (where T is a surface termination) were synthesized-as confirmed by Xray diffraction-from their corresponding MAX phase precursors (Nb 0.8 ,Ti 0.2 ) 4 AlC 3 and (Nb 0.8 ,Zr 0.2 ) 4 AlC 3 . This is the first report on a Zr-containing MXene. Intercalation of Li ions into these two compositions, and Nb 4 C 3 T x was studied to determine the potential of those materials for energy storage applications. Lithiation and delithiation peaks at 2.26 and 2.35 V, respectively, appeared in the case of Nb 4 C 3 T x , but were not present in Nb 2 CT x . After 20 cycles at a rate of C/4, the specific capacities of (Nb 0.8 ,Ti 0.2 ) 4 C 3 T x and (Nb 0.8 ,Zr 0.2 ) 4 C 3 T x were 158 and 132 mAh/g, respectively, both slightly lower than the capacity of Nb 4 C 3 T x .
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