Materials by Design: Tailored Morphology and Structures of Carbon Anodes for Enhanced Battery Safety.

Next-generation Li-ion battery technology awaits materials that not only store more electrochemical energy at finite rates but also exhibit superior control over side reactions and better thermal stability. Herein, we hypothesize that designing an appropriate particle morphology can provide a well-balanced set of physicochemical interactions. Given the anode-centric nature of primary degradation modes, we investigate three different carbon particles-commercial graphite, spherical carbon, and spiky carbon-and analyze the correlation between particle geometry and functionality. Intercalation dynamics, side reaction rates, self-heating, and thermal abuse behavior have been studied. It is revealed that the spherical particle outperforms an irregular one (commercial graphite) under thermal abuse conditions, as it eliminates unstructured inhomogeneities. A spiky particle with ordered protrusions exhibits smaller intercalation resistance and attenuated side reactions, thus outlining the benefits of controlled stochasticity. Such findings emphasize the importance of tailoring particle morphology to proffer selectivity among multimodal interactions.