Extending the energy-power balance of Li-ion batteries using graded electrodes with precise spatial control of local composition

Commercial Li-ion cell electrodes comprise a random mix of the constituent materials largely unchanged for more than three decades. During fast charge/discharge, electrode-scale Li-ion concentration gradients develop, along with a spatially heterogeneous distribution of overpotential, utilization and degradation of active material, which ultimately restricts the range of realizable energy-power combinations. We expand energy-power characteristics and reduce cell degradation rate using electrodes that are compositionally graded at the microscale to homogenize active material utilization. Trapezoidal-graded composition LiFePO4 cathodes, enabled by a layer-by-layer deposition technique, are compared with conventional electrodes: at an energy density of 500 Wh L−1 the best graded electrode design increased power density from approximately 100 W L−1 to 630 W L−1, while at a power density of 300 W L−1, the energy density increased from approximately 420 Wh L−1 to 600 Wh L−1. The results highlight the potential for new manufacturing approaches and electrode designs to provide performance enhancements for existing and future Li ion battery chemistries.