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.
|Journal||Advanced Functional Materials|
|Publication status||Published - 2021 Jan 11|
Bibliographical noteFunding Information:
J.H. and J.P. contributed equally to this work. Support from the Advanced Battery Materials Research (BMR) Program, in particular David Howell and Tien Duong, of the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, is gratefully acknowledged. S.‐M.B at Brookhaven National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the DOE through the BMR Program, including the Battery500 Consortium under contract DE‐SC0012704. This work made use of the EPIC facility at Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS 2025633); and the MRSEC program (NSF DMR‐1720139) at the Materials Research Center. The work by Y.K. was supported by the 2020 Research Fund (1.200070.01) of UNIST (Ulsan National Institute of Science & Technology). This research used resources of the Advanced Photon Source, a DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE‐AC02‐06CH11357. The XAS research used beamline 7‐BM (QAS) of the National Synchrotron Light Source II, a DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704. The submitted manuscript was created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science Laboratory, is operated under Contract No. DE‐AC02‐06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid‐up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government.
© 2020 Wiley-VCH GmbH
All Science Journal Classification (ASJC) codes
- Materials Science(all)
- Condensed Matter Physics