Although lithium-ion batteries (LIBs) have been currently the most reliable energy storage devices, further advances are still required to fulfill the rapidly growing market demand for larger-scale power supply systems. Accordingly, tremendous research efforts have been made to develop high-capacity anode materials to replace widely commercialized graphite anode materials having a limited theoretical capacity of ~372 mAh g-1. As an efficient strategy to enhance reaction kinetics for performance improvement, various electrode materials have been fabricated in nanoscale. Unexpectedly, the charge storage behaviors in the nanoscale are different from that of conventional micron-sized materials. A significant number of recently developed anode materials exhibit anomalously high reversible capacity exceeding the theoretical value based on conventional charge storage mechanism of insertion, alloying, and conversion reaction. Some of these materials even deliver more than two or three times higher capacity than graphite anode materials, over 1000 mAh g-1. Therefore, exploring the abnormal charge storage behavior and utilizing the new reactions could bring astonishing advances of current LIBs technology to the next level. Herein, the origins of extra capacity over theoretical value in some nanosized anode materials are investigated through systematic analyses, including in-depth synchrotron-based characterization techniques, computer simulation, and electrochemical tests. As so, it was discovered that materials, which were considered electrochemically inactive, reversibly participate in electrochemical reactions in nanoscale. Additionally, a new structural design strategy for utilizing the unconventional charge storage reaction will be provided. The present works will provide novel insight into the new paradigm of ion storage in nanostructured anode materials and enable the innovative design of electrode materials for next-generation LIBs. More details will be present at the time of the meeting.

Anomalous Li storage behavior of anode materials for next-generation Li batteries

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