JongTae Yoo

Flexible/shape-versatile, bipolar all-solid-state lithium-ion batteries prepared by multistage printing

Bipolar all-solid-state lithium-ion batteries (LIBs) have attracted considerable attention as a promising approach to address the ever-increasing demand for high energy and safety. However, the use of (sulfide- or oxide-based) inorganic solid electrolytes, which have been the most extensively investigated electrolytes in LIBs, causes problems with respect to mechanical flexibility and form factors in addition to their longstanding issues such as chemical/electrochemical instability, interfacial contact resistance and manufacturing processability. Here, we develop a new class of flexible/shape-versatile bipolar all-solid-state LIBs via ultraviolet (UV) curing-assisted multistage printing, which does not require the high-pressure/high-temperature sintering processes adopted for typical inorganic electrolyte-based all-solid-state LIBs. Instead of inorganic electrolytes, a flexible/nonflammable gel electrolyte consisting of a sebaconitrile-based electrolyte and a semi-interpenetrating polymer network skeleton is used as a core element in the printed electrodes and gel composite electrolytes (GCEs, acting as an ion-conducting separator membrane). Rheology tuning (toward thixotropic fluid behavior) of the electrode and GCE pastes, in conjunction with solvent-drying-free multistage printing, enables the monolithic integration of in-series/in-plane bipolar-stacked cells onto complex-shaped objects. Because of the aforementioned material and process novelties, the printed bipolar LIBs show exceptional flexibility, form factors, charge/discharge behavior and abuse tolerance (nonflammability) that far exceed those achievable with inorganic-electrolyte-based conventional bipolar cell technologies.

Molecularly designed, dual-doped mesoporous carbon/SWCNT nanoshields for lithium battery electrode materials

Formidable challenges facing lithium-ion rechargeable batteries, which involve performance degradations and safety failures during charge/discharge cycling, mostly arise from electrode–electrolyte interface instability. Here, as a polymeric ionic liquid (PIL)-mediated interfacial control strategy to address this long-standing issue, we demonstrate a new class of molecularly designed, ion/electron-conductive nanoshields based on single-walled carbon nanotube (SWCNT)-embedded, dual-doped mesoporous carbon (referred to as “SMC”) shells for electrode materials. The SMC shell is formed on cathode materials through solution deposition of the SWCNT/PIL mixture and subsequent carbonization. The PIL (denoted as “PVIm[DS]”) synthesized in this study consists of poly(1-vinyl-3-ethylimidazolium) cations and dodecyl sulfate counter anions, whose molecular structures are rationally designed to achieve the following multiple functions: (i) precursor for the conformal/continuous nanothickness carbon shell, (ii) dual (N and S)-doping source, (iii) porogen for the mesoporous structure, and (iv) SWCNT dispersant. Driven by such chemical/structural uniqueness, the SMC shell prevents direct exposure of cathode materials to bulk liquid electrolytes while facilitating redox reaction kinetics. As a consequence, the SMC-coated cathode materials enable significant improvements in cell performance and also thermal stability. We envision that the SMC shell can be suggested as a new concept of effective and versatile surface modification strategy for next-generation high-performance electrode materials.

Nanocarbons in Li-Ion Batteries

The ever-increasing demand for advanced power sources with higher energy density and various form factors strongly pushes us to search for new battery materials and structures beyond current state-of-the-art Li-ion batteries (LIBs). Recent progress in nanoscience and nanotechnology suggests opportunities to develop novel electrode materials and architectures for next-generation Li-ion batteries. Among numerous nanomaterials reported to date, nanocarbons have garnered considerable attention as a promising battery element to enrich electrode chemistry and materials. Of various nanocarbons, carbon nanotube and graphene exhibit outstanding electrical and mechanical properties, large surface area, and unique structural characteristics, which thus bring significant improvements in electrochemical performance and flexibility/design diversity of lithium-based power sources. Here, we describe current status and challenges of nanocarbons in LIBs, with a particular focus on their potential application to anode materials, conductive agents, current collectors, and structure-directing substances for electrodes.

One-pot surface engineering of battery electrode materials with metallic SWCNT-enriched, ivy-like conductive nanonets

A longstanding challenge facing energy conversion/storage materials is their low electrical conductivity, which often results in unwanted sluggish electrochemical reactions. Here, we demonstrate a new class of one-pot surface engineering strategy based on metallic single-walled carbon nanotube (mSWCNT)-enriched, ivy-like conductive nanonets (mSC nanonets). The mSC nanonets are formed on the surface of electrode materials through a poly(9,9-di-n-octylfluorenyl-2,7-diyl) (PFO)-assisted sonication/filtration process. PFO is known as a dispersant for SWCNTs that shows a higher affinity for semiconducting SWCNTs (sSWCNTs) than for mSWCNTs. Driven by this preferential affinity of PFO, sSWCNTs are separated from mSWCNTs in the form of sSWCNT/PFO hybrids, and the resulting enriched mSWCNTs are uniformly deposited on electrode materials in the form of ivy-like nanonets. Various electrode materials, including lithium-ion battery cathodes/anodes and perovskite catalysts, are chosen to explore the feasibility of the proposed concept. Due to their ivy-like conductive network, the mSC nanonets increase the electronic conductivity of the electrode materials without hindering their ionic transport, eventually enabling significant improvements in their redox reaction rates, charge/discharge cyclability, and bifunctional electrocatalytic activities. These exceptional physicochemical advantages of the mSC nanonets, in conjunction with the simplicity/versatility of the one-pot surface engineering process, offer a new and facile route to develop advanced electrode materials with faster electrochemical reaction kinetics.