Recrystallization prohibiting lithium dendrites

Demand for lithium-ion batteries (LIBs) is increasing owing to the expanding use of electrical vehicles and stationary energy storage. Efficient and closed-loop battery recycling strategies are therefore needed, which will require recovering materials from spent LIBs and reintegrating them into new batteries. In this Review, we outline the current state of LIB recycling, evaluating industrial and developing technologies. Among industrial technologies, pyrometallurgy can be broadly applied to diverse electrode materials but requires operating temperatures of over 1,000 °C and therefore has high energy consumption. Hydrometallurgy can be performed at temperatures below 200 °C and has material recovery rates of up to 93% for lithium, nickel and cobalt, but it produces large amounts of wastewater. Developing technologies such as direct recycling and upcycling aim to increase the efficiency of LIB recycling and rely on improved pretreatment processes with automated disassembly and cleaner mechanical separation. Additionally, the range of materials recovered from spent LIBs is expanding from the cathode materials recycled with established methods to include anode materials, electrolytes, binders, separators and current collectors. Achieving an efficient recycling ecosystem will require collaboration between recyclers, battery manufacturers and electric vehicle manufacturers to aid the design and automation of battery disassembly lines.

The discovery of Nb-W-O materials years ago marks the milestone of charging a lithium-ion battery in minutes. Nevertheless, for many applications, charging lithium-ion battery within one minute is urgently demanded, the bottleneck of which largely lies in the lack of fundamental understanding of Li⁺ storage mechanisms in these materials. Herein, by visualizing Li⁺ intercalated into representative Nb₁₆W₅O₅₅, we find that the fast-charging nature of such material originates from an interesting rate-dependent lattice relaxation process associated with the Jahn-Teller effect. Furthermore, in situ electron microscopy further reveals a directional, [010]-preferred Li⁺ transport mechanism in Nb₁₆W₅O₅₅ crystals being the “bottleneck” toward fast charging that deprives the entry of any desolvated Li⁺ through the prevailing non-(010) surfaces. Hence, we propose a machine learning-assisted interface engineering strategy to swiftly collect desolvated Li⁺ and relocate them to (010) surfaces for their fast intercalation. As a result, a capacity of ≈ 116 mAh g⁻¹ (68.5% of the theoretical capacity) at 80 C (45 s) is achieved when coupled with a Li negative electrode.