Carbon binder domain networks and electrical conductivity in lithium-ion battery electrodes: A critical review

In a drive to increase Li-ion battery energy density, as well as support faster charge discharge speeds, electronic conductivity networks require increasingly efficient transport pathways whilst using ever decreasing proportions of conductive additive. Comprehensive understanding of the complexities of electronic conduction in lithium-ion battery electrodes is lacking in the literature. In this work we show higher electronic conductivities do not necessarily lead to higher capacities at high C-rates due to the complex interrelation between the electronically conducting carbon binder domain (CBD) and the ionic diffusion within electrodes. A wide body of literature is reviewed, encompassing the current maxims of percolation theory and conductive additives as well as the relationships between processing steps at each stage of electrode manufacturing and formation of electronic conduction pathways. The state-of-the-art in electrode characterisation techniques are reviewed in the context of providing a holistic and accurate understanding of electronic conductivity. Literature regarding the simulation of electrode structures and their electronic properties is also reviewed. This review presents the first comprehensive survey of the formation of electronic conductivity networks throughout the CBD in battery electrodes, and demonstrates a lack of understanding regarding the most optimum arrangement of the CBD in the literature. This is further explored in relation to the long-range and short-range electrical contacts within a battery electrode which represent the micron level percolation network and the submicron connection of CBD to active material respectively. A guide to future investigations into CBD including specific characterisation experiments and simulation approaches is suggested. We conclude with suggestions on reporting important metrics such as robust electrical characterisation and the provision of metrics to allow comparison between studies such as aerial current density. Future advances in characterisation, simulation and experimentation will be able to provide a more complete understanding if research can be quantitatively compared.