The introduction of structural energy storage devices into emerging markets, such as electric vehicles, is predominately hindered by weak energy density, safety concerns, and immaturity of the field in materials. Herein, fabrication and testing of a freeze-resistant, multifunctional quasi-solid-state zinc−sulfur battery (ZnS) are reported. To this end, an electrostatic spray coating technique was used to deposit a thin layer of sulfur on the highly porous, unidirectional activated carbon nanofibers (A-CNFs) as a load-bearing cathode. This technique could fill micro-and mesopores, and microsized channels with sulfur, achieving an extensive sulfur loading of 60 wt %. Several drawbacks of structural energy storage devices (applicability under varied climate conditions, poor electrochemical performance and mechanical properties) are addressed by initiating an antifreezing hydrogel electrolyte with a failure strain of over 200%. This electrolyte possesses ethylene glycol and an I 2 additive as an antifreezing agent and redox mediator, respectively. The as-assembled ZnS battery offers a high energy density of 283 Wh/kg based on the CNF-S cathode (149 Wh/ kg based on the ZnS cell) and mechanical properties beyond state-of-the-art structural energy storage devices with a tensile strength of 377 MPa, Young's modulus of 16.7 GPa, and energy-to-failure of 4.5 MJ/m 3 . The electrochemomechanical properties of the ZnS battery were also investigated to elucidate the effects of electrochemical energy storage on mechanical properties and vice versa. Overall, the ZnS battery outperforms state-of-the-art structural energy storage devices in terms of energy storage and load-bearing capabilities.

This study presents the design and fabrication of the inaugural kirigami-inspired stretchable zinc–sulfur (Zn–S) battery with remarkable electro-chemo-mechanical properties.