Rational Design of Dendritic Phase‐Pure Tin Antimonide Intermetallic Film‐Based Negatrodes for Commercially‐Viable Flexible Sodium‐Ion Pouch Cell Battery

Abstract Exploiting the ability to directly deposit larger‐sized, flexible, alloying‐type sodium‐ion battery electrodes without the need of additional inactive components and processing steps is a strategic way to achieve higher gravimetric capacities which will be suitable for commercial‐level sodium‐ion (SIB) pouch cell manufacturing. In this regard, a simple, template‐free electroplating protocol is reported for designing phase‐pure tin antimonide (TA)‐based negatrode. An optimum control over the potentiostatic electroplating parameters allows the preferential formation of dendritic nanostructures over an electroplated foam‐based current collector. The prepared negatrode and Mn‐based Prussian blue analog positrode in full coin cell format deliver an average nominal working voltage of 3.0 V with a discharge energy density of 342 Wh kg −1 . In single‐layer full pouch cell format, an 8.01 mAh capacity (89.89 mAh g −1 , 593.3 µAh cm −2 ) is achieved at an undeformed state and 97.12% capacity is retained at 180° bend condition. In multi‐layer full pouch cell format, a 35.86 mAh capacity (80.58 mAh g −1 , 531.2 µAh cm −2 ) is achieved with 62.77% capacity retention after 200 cycles (0.125 C). The results of this work showcase how a simple, template free, aqueous electrolyte based electroplating protocol can be developed for the direct fabrication of large‐sized, flexible, alloying‐type negatrodes for commercial SIB pouch cells.