Conducting Polymer-Skinned Electroactive Materials of Lithium-Ion Batteries: Ready for Monocomponent Electrodes without Additional Binders and Conductive Agents

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

Activity-Durability Coincidence of Oxygen Evolution Reaction in the Presence of Carbon Corrosion: Case Study of MnCo₂O₄ Spinel with Carbon Black

Highly oxygen evolution reaction (OER)-active electrocatalysts often exhibit improved OER durability in the presence of carbon corrosion or oxidation (COR) in the literature. The activity-durability coincidence of OER electrocatalysts was theoretically understood by preferential depolarization in galvanostatic situations. At constant-current conditions for a system involving multiple reactions that are independent and competitive, the overpotential is determined most dominantly by the most facile reaction so that the most facile reaction is responsible for a dominant portion of the overall current. Therefore, higher OER activity improves durability by mitigating the current responsible for COR. The activity-durability coincidence was then proved experimentally by comparing between two catalysts of the same chemical identity (MnCo₂O₄) in different dimensions (5 and 100 nm in size). Carbon corrosion responsible for inferior durability was suppressed in the smaller-dimension catalyst (MnCo₂O₄ in 5 nm) having more numbers of active sites per a fixed mass