Reversible Li-ion conversion reaction for a TixGe alloy in a Ti/Ge multilayer

Chen, Xiao; Fister, Tim T.; Esbenshade, Jennifer; Shi, Bing; Hu, Xianyi; Wu, Jinsong; Gewirth, Andrew A.; Bedzyk, Michael J.; Fenter, Paul

doi:10.1021/acsami.6b14783

Title: Reversible Li-ion conversion reaction for a Ti_xGe alloy in a Ti/Ge multilayer

Abstract

Group IV inter-metallics electrochemically alloy with Li with stoichiometries as high as Li_4.4M (M=Si, Ge, Sn or Pb). Furthermore, this provides the second highest known specific capacity (after pure lithium metal) for lithium ion batteries, but the dramatic volume change during cycling greatly limits their use as anodes in Li-ion batteries. We describe an approach to overcome this limitation by constructing electrodes using a Ge/Ti multilayer architecture. In operando X-ray reflectivity and ex situ transmission electron microscopy are used to characterize the hetero-layer structure at various lithium stoichiometries along a lithiation/delithiation cycle. The as-deposited multilayer spontaneously forms a one-dimensional Ti_xGe/Ti/Ti_xGe core-shell planar structure embedded in a Ge matrix. The interfacial Ti_xGe alloy is observed to be electrochemically active and exhibits reversible phase separation (i.e. a conversion reaction). Including the germanium components, the overall multilayer structure exhibits a 2.3-fold reversible vertical expansion and contraction and is shown to have improved capacity and capacity retention with respect to a Ge film with equivalent active material thickness.

Authors:

Chen, Xiao ^[1]; Fister, Tim T. ^[2]; Esbenshade, Jennifer ^[3]; Shi, Bing ^[2]; Hu, Xianyi ^[4]; Wu, Jinsong ^[4];

^[3];

^[4];

^[2]

Argonne National Lab. (ANL), Lemont, IL (United States); Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Univ. of Illinois Urbana-Champaign, Champaign, IL (United States)
Northwestern Univ., Evanston, IL (United States)

Publication Date:: Mon Feb 13 00:00:00 EST 2017

Research Org.:: Argonne National Laboratory (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1371561

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: ACS Applied Materials and Interfaces

Additional Journal Information:: Journal Volume: 9; Journal Issue: 9; Journal ID: ISSN 1944-8244

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 25 ENERGY STORAGE; Ge/Ti alloy; germanium; Li-ion battery; Patterson function; X-ray reflectivity; multilayer; thin film

Citation Formats


                    Chen, Xiao, Fister, Tim T., Esbenshade, Jennifer, Shi, Bing, Hu, Xianyi, Wu, Jinsong, Gewirth, Andrew A., Bedzyk, Michael J., and Fenter, Paul. Reversible Li-ion conversion reaction for a TixGe alloy in a Ti/Ge multilayer.  United States: N. p., 2017. 
Web.  doi:10.1021/acsami.6b14783.

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                    Chen, Xiao, Fister, Tim T., Esbenshade, Jennifer, Shi, Bing, Hu, Xianyi, Wu, Jinsong, Gewirth, Andrew A., Bedzyk, Michael J., & Fenter, Paul. Reversible Li-ion conversion reaction for a TixGe alloy in a Ti/Ge multilayer.  United States.  https://doi.org/10.1021/acsami.6b14783

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                    Chen, Xiao, Fister, Tim T., Esbenshade, Jennifer, Shi, Bing, Hu, Xianyi, Wu, Jinsong, Gewirth, Andrew A., Bedzyk, Michael J., and Fenter, Paul. Mon .  
"Reversible Li-ion conversion reaction for a TixGe alloy in a Ti/Ge multilayer".  United States.  https://doi.org/10.1021/acsami.6b14783.  https://www.osti.gov/servlets/purl/1371561.

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@article{osti_1371561,

  title        = {Reversible Li-ion conversion reaction for a TixGe alloy in a Ti/Ge multilayer},

  author       = {Chen, Xiao and Fister, Tim T. and Esbenshade, Jennifer and Shi, Bing and Hu, Xianyi and Wu, Jinsong and Gewirth, Andrew A. and Bedzyk, Michael J. and Fenter, Paul},

  abstractNote = {Group IV inter-metallics electrochemically alloy with Li with stoichiometries as high as Li4.4M (M=Si, Ge, Sn or Pb). Furthermore, this provides the second highest known specific capacity (after pure lithium metal) for lithium ion batteries, but the dramatic volume change during cycling greatly limits their use as anodes in Li-ion batteries. We describe an approach to overcome this limitation by constructing electrodes using a Ge/Ti multilayer architecture. In operando X-ray reflectivity and ex situ transmission electron microscopy are used to characterize the hetero-layer structure at various lithium stoichiometries along a lithiation/delithiation cycle. The as-deposited multilayer spontaneously forms a one-dimensional TixGe/Ti/TixGe core-shell planar structure embedded in a Ge matrix. The interfacial TixGe alloy is observed to be electrochemically active and exhibits reversible phase separation (i.e. a conversion reaction). Including the germanium components, the overall multilayer structure exhibits a 2.3-fold reversible vertical expansion and contraction and is shown to have improved capacity and capacity retention with respect to a Ge film with equivalent active material thickness.},

  doi          = {10.1021/acsami.6b14783},

  journal      = {ACS Applied Materials and Interfaces},

  number       = 9,

  volume       = 9,

  place        = {United States},

  year         = {Mon Feb 13 00:00:00 EST 2017},

  month        = {Mon Feb 13 00:00:00 EST 2017}

}

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Works referencing / citing this record:

Sputtered Ge/Si Nanocomposite Films as High Performance Anode Materials for Lithium-Ion Battery
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Liu, Biaobiao; Chen, Anran; Wang, Rongfei
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Title: Reversible Li-ion conversion reaction for a TixGe alloy in a Ti/Ge multilayer

Abstract

Citation Formats

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Title: Reversible Li-ion conversion reaction for a Ti_xGe alloy in a Ti/Ge multilayer

Nanocrystalline and Thin Film Germanium Electrodes with High Lithium Capacity and High Rate Capabilities
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Study of Germanium as Electrode in Thin-Film Battery
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Tin-Nanoparticles Encapsulated in Elastic Hollow Carbon Spheres for High-Performance Anode Material in Lithium-Ion Batteries
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Electrochemical Reaction of Lithium with Nanostructured Silicon Anodes: A Study by In-Situ Synchrotron X-Ray Diffraction and Electron Energy-Loss Spectroscopy
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Mesoporous germanium as anode material of high capacity and good cycling prepared by a mechanochemical reaction
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