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New High-Performance Pb-Based Nanocomposite Anode Enabled by Wide-Range Pb Redox and Zintl Phase Transition
Authors:Jinhyup Han  Jehee Park  Seong-Min Bak  Seoung-Bum Son  Jihyeon Gim  Cesar Villa  Xiaobing Hu  Vinayak P Dravid  Chi Cheung Su  Youngsik Kim  Christopher Johnson  Eungje Lee
Affiliation:1. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, 60439 USA;2. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, 60439 USA

School of Energy & Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919 South Korea;3. Chemistry Division, Brookhaven National Laboratory, Upton, NY, 11973 USA;4. Department of Materials Science and Engineering, Northwestern University, Evanston, IL, 60208 USA;5. Department of Materials Science and Engineering, Northwestern University, Evanston, IL, 60208 USA

The NUANCE Center, Northwestern University, Evanston, IL, 60208 USA;6. School of Energy & Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919 South Korea

Abstract: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.
Keywords:alloying  conversion  lead (Pb) anode  lithium-ion batteries  Zintl phase
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