Fundamental Studies of Discharge Mechanism and Capacity Limits of Lead Acid Battery Electrodes

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Long-duration energy storage provides key benefits such as consistent power supply during periods of high demand for grid reliability and flexibility. For environmental benefits, it allows for more renewable energy integration and helps reduce reliance on fossil fuels to lower greenhouse gas emission. Lead batteries have the economic potential to continue serving as an important energy storage technology for a decarbonized sustainable energy future given they are earth-abundant, inexpensive, and 99% recyclable. Advancing the design of lead batteries with higher material utilization, fast recharge rates, and long-cycle life requires a fundamental understanding of the electrochemical and chemical processes taking place at the atomic and molecular scales. In this work, we will discuss how the use of well-defined electrode interfaces allows us to gain insights into the fundamental limits of discharge capacity and recharge rates. We were able to unveil the relationships between discharge rates and PbSO4 particle size/layer thickness that ultimately governs the maximum discharge capacity accessible as a function of discharge rate on both the negative and positive lead electrodes. This data helped us develop a mathematical model that captures the key processes concerning lead ion and (bi)sulfate ion gradients coupled to nucleation and growth that explain, from first principles, the origin of the well-known empirical Peukert law. In this context, exploring how variables such as acid concentration, temperature, and the presence of lignosulfonate additives in the electrolyte further influence discharge capacity allows us to understand how thermodynamic, kinetic, and even mass transport play a huge role in governing the accessible capacity from the electrodes. This study paves the way for a deeper understanding of the variables that are most important in improving the discharge capacity of lead-acid batteries, and thus batteries that can be utilized at their full potential.