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The present article introduces a strategy for controlling oxidation and reduction reactions within polymer electrolyte membrane (PEM) networks as a means of enhancing storage capacity through the complexation of dissociated lithium cations with multifunctional groups of the polymer network. Specifically, co-polymer networks based on polysulfide (PS) and polyoxide (PO) precursors, photo-cured in the presence of succinonitrile (SCN) and lithium bis(trifluoro methane sulfonyl imide) (LiTFSI) salt, exhibited ionic conductivity on the order of mid 10−4 S/cm at ambient temperature in the 30/35/35 (weight %) composition. Lithium titanate (LTO, Li4Ti5O12) electrode was chosen as an anode (i.e., a potential source of Li ions) against lithium iron phosphate (LFP, LiFePO4) cathode in conjunction with polysulfide-co-polyoxide dual polyelectrolyte networks to control viscosity for 3D printability on conformal surfaces of drone and aeronautic vehicles. It was found that the PS-co-PO dual network-based polymer electrolyte containing SCN plasticizer and LiTFSI salt exhibited extra storage capacity (i.e., specific capacity of 44 mAh/g) with the overall specific capacity of 170 mAh/g (i.e., for the combined LTO electrode and PEM) initially that stabilized at 153 mAh/g after 50th cycles with a reasonable capacity retention of over 90% and Coulombic efficiency of over 99%. Of particular interest is the observation of the improved electrochemical performance of the polysulfide-co-polyoxide electrolyte dual-network relative to that of the polyoxide electrolyte single-network. 

The year 1975 can be claimed to be the year of inception for the research and development of solid polymer electrolytes (SPEs) for Lithium-Ion Batteries (LIB), when the ionic conductivity of polyethylene oxide–alkaline metal ion complex was found by Peter Wright from the University of Sheffield. However, SPE research has undergone a leapfrog development, with conductivity values improving from 1 × 10–7 S·cm−1 to 1 × 10– 1 S·cm−1. The seed of development of SPEs spurs from the need for introducing design freedom to battery structures as well as the need for leak-proof electrolytes, greater operational safety, higher energy density, and other considerations. While the benefits of SPEs are evident, poor interfacial contact is a major factor limiting their application. This review presents the history of SPEs and shows how the additive manufacturing (AM) could prove beneficial for the improvement of performance and the functional implementation of SPEs. While the article articulates a technical review of additively manufactured SPEs, it also provides a lab-to-market perspective that could aid in shaping the future of green technology in energy storage. It also aims to provide an overall picture about the evolution and diversity of research advances in the development of greener SPEs through AM technology.