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

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

doi:10.1002/adfm.202005362

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

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

Department of Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

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 Li_yPb 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.

Original language	English
Article number	2005362
Journal	Advanced Functional Materials
Volume	31
Issue number	2
DOIs	https://doi.org/10.1002/adfm.202005362
Publication status	Published - 2021 Jan 11

Bibliographical note

Funding 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.

Publisher Copyright:
© 2020 Wiley-VCH GmbH

All Science Journal Classification (ASJC) codes

Chemistry(all)
Materials Science(all)
Condensed Matter Physics

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/adfm.202005362

Cite this

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title = "New High-Performance Pb-Based Nanocomposite Anode Enabled by Wide-Range Pb Redox and Zintl Phase Transition",

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.",

author = "Jinhyup Han and Jehee Park and Bak, {Seong Min} and Son, {Seoung Bum} and Jihyeon Gim and Cesar Villa and Xiaobing Hu and Dravid, {Vinayak P.} and Su, {Chi Cheung} and Youngsik Kim and Christopher Johnson and Eungje Lee",

note = "Funding 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. Publisher Copyright: {\textcopyright} 2020 Wiley-VCH GmbH",

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doi = "10.1002/adfm.202005362",

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AU - Han, Jinhyup

AU - Park, Jehee

AU - Bak, Seong Min

AU - Son, Seoung Bum

AU - Gim, Jihyeon

AU - Villa, Cesar

AU - Hu, Xiaobing

AU - Dravid, Vinayak P.

AU - Su, Chi Cheung

AU - Kim, Youngsik

AU - Johnson, Christopher

AU - Lee, Eungje

N1 - Funding 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. Publisher Copyright: © 2020 Wiley-VCH GmbH

PY - 2021/1/11

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N2 - 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.

AB - 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.

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

Abstract

Bibliographical note

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UN SDGs

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