In Situ Inorganic and Polymer Synthesis for Conformal Hybrid Sulfide-Type Solid State Electrolytes

Hybrid inorganic-polymer materials are promising candidates to solve a variety of challenges, particularly in lithium metal batteries. However, traditional synthetic paradigms for hybrid materials require the separate synthesis of the inorganic and polymer, presenting major challenges toward controlling the microstructure of the material which can greatly affect the performance of the material. In this study, we develop a class of hybrid sulfide-polymer materials through an innovative one-pot, in situ synthetic paradigm. Utilizing dichloroethane (DCE) as a test case, we show that both polymer and inorganic form and present a controlled, homogeneous distribution of the inorganic and polymer. At certain ratios, we find evidence of a covalent linkage between the inorganic and polymer. We showcased the material in a lithium metal battery where our in situ material has improved mechanical properties and superior ionic conductivity and cycling performance against Li–metal in comparison to an ex situ polymer + sulfide control. Additionally, the chemical space of this reaction is vast, and we demonstrate covalent linkages in a variety of other monomers in addition to DCE. Our work will change the synthetic paradigm for hybrid inorganic-polymer electrolytes and open a pathway for utilization of these materials in other applications.