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Hysteresis is a general phenomenon regularly observed in measurements ofvarious materials properties such as magnetism, elasticity, capillary pressure,adsorption, battery voltage etc. Usually, the hysteretic behaviour is anintrinsic property that cannot be avoided or circumvented in dynamic operationof the system. Here we show, however, that at least as regards the hystereticbehaviour of phase-separating battery materials, one can enter (deeply) intothe hysteretic loop in specific, yet realistic, transient operating conditions.Within the hysteretic loop a (significant) portion of particle populationresides in an intraparticle phase separated state. Interestingly, thetransition to the more conventional interparticle phase separation state foundoutside the hysteretic loop is very slow. Further, we establish a directinterrelation between the intraparticle phase separated electrode state andaltered electric response of the electrode, which significantly impacts DC andAC characteristics of the battery. The experimental evidence of entering thehysteretic loop and the resulting altered response of the battery are explainedbased on thermodynamic reasoning, advanced modelling and insightfulexperiments. We believe that the understanding of this phenomenon will helpoptimise the diagnostics and monitoring of batteries, while also providingpertinent motivation for the enhancement of battery design and performance.

Entering voltage hysteresis in phase separating materials: revealing the  thermodynamic origin of a newly discovered phenomenon and its impact on the  electric response of a battery