Publication date: 10th April 2024
Fast charging and high power delivery in rechargeable battery electrodes requires rapid ionic and electronic transport. In addition, long-term cycling demands electrode stability and the reversibility of ion insertion and extraction. Two structural families that satisfy these criteria are the crystallographic shear structures and bronze-like phases that are found in many niobium-containing binary and ternary early transition metal oxides. Several members of these large families have demonstrated the ability to store large quantities of lithium at rates well above 1C up to and above 20C; these rates are accessible without nanostructuring.
The maximum power output and minimum charging time of a lithium-ion battery – key parameters for its use in, for example, transportation applications – depend on mixed ionic–electronic diffusion. While the discharge/charge rate and capacity can be tuned by varying the composite electrode structure, ionic transport within the active particles represents a fundamental limitation. Thus, to achieve high rates, particles are frequently reduced to nanosize dimensions despite this being disadvantageous in terms of volumetric packing density as well as cost, stability, and sustainability considerations. As an alternative to nanoscaling, we show that complex niobium oxides with topologically frustrated polyhedral arrangements and dense micron-scale particle morphologies can rapidly and reversibly intercalate large quantities of lithium. Multielectron redox, buffered volume expansion, and extremely fast lithium transport approaching that of a liquid lead to extremely high volumetric capacities and rate performance as reported in both crystallographic shear structure and bronze-like niobium-based oxides[1–6]. The active materials offer new strategies toward designing electrodes with advantages in energy density, scalability, electrode architecture/complexity and cost as alternatives to graphite and Li4Ti5O12.
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