New High‐Performance Pb‐Based Nanocomposite Anode Enabled by Wide‐Range Pb Redox and Zintl Phase Transition

This paper describes a new, high‐performance, Pb‐based nanocomposite anode material for lithium‐ion batteries. A unique nanocomposite structure of Pb@PbO core‐shell nanoparticles in a carbon matrix is obtained by using a simple high‐energy ball milling method using the low‐cost starting materials PbO and carbon black. Electrochemical performance tests show its excellent reversible capacity (≈600 mAh g−1) and cycle stability (92% retention at 100th cycle), which are one of the best values reported for Pb‐based anodes in the literature. Synchrotron X‐ray diffraction and absorption techniques revealed the detailed lithium storage mechanism that can be highlighted with the unexpectedly wide reversible Pb redox range (between Pb2+ and Pb4−) and the evolution of Zintl‐type LiyPb structures during the electrochemical lithium reaction. The results provide new insights into the lithium storage mechanism of these Pb‐based materials and their potential as low‐cost, high‐performance anodes. A novel high‐performance Pb@PbOC nanocomposite anode material is synthesized via a simple high‐energy ball milling process using low‐cost lead oxide and carbon as starting materials. This report covers the unique nanocomposite structure that enables unprecedentedly high electrochemical performance and the detailed lithium storage mechanism that unlocks the prospects of new conversion‐alloying‐based anode materials for practical applications.