A facile approach to the surface modification of spinel LiNi 0.5 Mn 1.5 O 4 (LNMO) cathode active materials for high-voltage lithium ion batteries is demonstrated. This strategy is based on nanoarchitectured polyimide (PI) gel polymer electrolyte (GPE) coating. The PI coating layer successfully wrapped a large area of the LNMO surface via thermal imidization of 4-component (pyromellitic dianhydride/biphenyl dianhydride/phenylenediamine/oxydianiline) polyamic acid. In comparison to conventional metal oxide-based coatings, distinctive features of the unusual PI wrapping layer are the highly continuous surface coverage with nanometre thickness ($10 nm) and the provision of facile ion transport. The nanostructure-tuned PI wrapping layer served as an ionconductive protection skin to suppress the undesired interfacial side reactions, effectively preventing the direct exposure of the LNMO surface to liquid electrolyte. As a result, the PI wrapping layer played a crucial role in improving the high-voltage cell performance and alleviating the interfacial exothermic reaction between charged LNMO and liquid electrolyte. Notably, the superior cycle performance (at 55 C) of the PI-wrapped LNMO (PI-LNMO) was elucidated in great detail by quantitatively analyzing manganese (Mn) dissolution, cell impedance, and chemical composition (specifically, lithium fluoride (LiF)) of byproducts formed on the LNMO surface.

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Rapid growth of mobile and even wearable electronics is in pursuit of high-energy-density lithium-ion batteries. One simple and facile way to achieve this goal is the elimination of nonelectroactive components of electrodes such as binders and conductive agents. Here, we present a new concept of monocomponent electrodes comprising solely electroactive materials that are wrapped with an insignificant amount (less than 0.4 wt %) of conducting polymer (PEDOT:PSS or poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate)). The PEDOT:PSS as an ultraskinny surface layer on electroactive materials (LiCoO2 (LCO) powders are chosen as a model system to explore feasibility of this new concept) successfully acts as a kind of binder as well as mixed (both electrically and ionically) conductive film, playing a key role in enabling the monocomponent electrode. The electric conductivity of the monocomponent LCO cathode is controlled by simply varying the PSS content and also the structural conformation (benzoid-favoring coil structure and quinoid-favoring linear or extended coil structure) of PEDOT in the PEDOT:PSS skin. Notably, a substantial increase in the mass-loading density of the LCO cathode is realized with the PEDOT:PSS skin without sacrificing electronic/ionic transport pathways. We envisage that the PEDOT:PSS-skinned electrode strategy opens a scalable and versatile route for making practically meaningful binder-/conductive agent-free (monocomponent) electrodes.

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