DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Stable metal battery anodes enabled by polyethylenimine sponge hosts by way of electrokinetic effects

Abstract

The cycle life and energy density of rechargeable metal batteries are largely limited by the dendritic growth of their metal anodes (lithium, sodium or zinc). Here we develop a three-dimensional cross-linked polyethylenimine lithium-ion-affinity sponge as the lithium metal anode host to mitigate the problem. We show that electrokinetic surface conduction and electro-osmosis within the high-zeta-potential sponge change the concentration and current density profiles, which enables dendrite-free plating/stripping of lithium with a high Coulombic efficiency at high deposition capacities and current densities, even at low temperatures. The use of a lithium-hosting sponge leads to a significantly improved cycling stability of lithium metal batteries with a limited amount of lithium (for example, the areal lithium ratio of negative to positive electrodes is 0.6) at a commercial-level areal capacity. We also observed dendrite-free morphology in sodium and zinc anodes, which indicates a broader promise of this approach.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Research Org.:
Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1497676
Grant/Contract Number:  
EE0007795; EE0007803
Resource Type:
Accepted Manuscript
Journal Name:
Nature Energy
Additional Journal Information:
Journal Volume: 3; Journal Issue: 12; Related Information: Supplementary information is available for this paper at https://doi.org/10.1038/s41560-018-0276-z; Journal ID: ISSN 2058-7546
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; 42 ENGINEERING; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Li, Guoxing, Liu, Zhe, Huang, Qingquan, Gao, Yue, Regula, Michael, Wang, Daiwei, Chen, Long-Qing, and Wang, Donghai. Stable metal battery anodes enabled by polyethylenimine sponge hosts by way of electrokinetic effects. United States: N. p., 2018. Web. doi:10.1038/s41560-018-0276-z.
Li, Guoxing, Liu, Zhe, Huang, Qingquan, Gao, Yue, Regula, Michael, Wang, Daiwei, Chen, Long-Qing, & Wang, Donghai. Stable metal battery anodes enabled by polyethylenimine sponge hosts by way of electrokinetic effects. United States. https://doi.org/10.1038/s41560-018-0276-z
Li, Guoxing, Liu, Zhe, Huang, Qingquan, Gao, Yue, Regula, Michael, Wang, Daiwei, Chen, Long-Qing, and Wang, Donghai. Mon . "Stable metal battery anodes enabled by polyethylenimine sponge hosts by way of electrokinetic effects". United States. https://doi.org/10.1038/s41560-018-0276-z. https://www.osti.gov/servlets/purl/1497676.
@article{osti_1497676,
title = {Stable metal battery anodes enabled by polyethylenimine sponge hosts by way of electrokinetic effects},
author = {Li, Guoxing and Liu, Zhe and Huang, Qingquan and Gao, Yue and Regula, Michael and Wang, Daiwei and Chen, Long-Qing and Wang, Donghai},
abstractNote = {The cycle life and energy density of rechargeable metal batteries are largely limited by the dendritic growth of their metal anodes (lithium, sodium or zinc). Here we develop a three-dimensional cross-linked polyethylenimine lithium-ion-affinity sponge as the lithium metal anode host to mitigate the problem. We show that electrokinetic surface conduction and electro-osmosis within the high-zeta-potential sponge change the concentration and current density profiles, which enables dendrite-free plating/stripping of lithium with a high Coulombic efficiency at high deposition capacities and current densities, even at low temperatures. The use of a lithium-hosting sponge leads to a significantly improved cycling stability of lithium metal batteries with a limited amount of lithium (for example, the areal lithium ratio of negative to positive electrodes is 0.6) at a commercial-level areal capacity. We also observed dendrite-free morphology in sodium and zinc anodes, which indicates a broader promise of this approach.},
doi = {10.1038/s41560-018-0276-z},
journal = {Nature Energy},
number = 12,
volume = 3,
place = {United States},
year = {Mon Nov 12 00:00:00 EST 2018},
month = {Mon Nov 12 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 258 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Metallic anodes for next generation secondary batteries
journal, January 2013

  • Kim, Hansu; Jeong, Goojin; Kim, Young-Ugk
  • Chemical Society Reviews, Vol. 42, Issue 23
  • DOI: 10.1039/c3cs60177c

Issues and challenges facing rechargeable lithium batteries
journal, November 2001

  • Tarascon, J.-M.; Armand, M.
  • Nature, Vol. 414, Issue 6861, p. 359-367
  • DOI: 10.1038/35104644

Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries
journal, October 2004


Lithium metal anodes for rechargeable batteries
journal, January 2014

  • Xu, Wu; Wang, Jiulin; Ding, Fei
  • Energy Environ. Sci., Vol. 7, Issue 2
  • DOI: 10.1039/C3EE40795K

An Artificial Solid Electrolyte Interphase with High Li-Ion Conductivity, Mechanical Strength, and Flexibility for Stable Lithium Metal Anodes
journal, December 2016

  • Liu, Yayuan; Lin, Dingchang; Yuen, Pak Yan
  • Advanced Materials, Vol. 29, Issue 10
  • DOI: 10.1002/adma.201605531

Poly(dimethylsiloxane) Thin Film as a Stable Interfacial Layer for High-Performance Lithium-Metal Battery Anodes
journal, October 2016


Interconnected hollow carbon nanospheres for stable lithium metal anodes
journal, July 2014

  • Zheng, Guangyuan; Lee, Seok Woo; Liang, Zheng
  • Nature Nanotechnology, Vol. 9, Issue 8
  • DOI: 10.1038/nnano.2014.152

A facile surface chemistry route to a stabilized lithium metal anode
journal, July 2017


Electrolyte additive enabled fast charging and stable cycling lithium metal batteries
journal, March 2017


Self-Formed Hybrid Interphase Layer on Lithium Metal for High-Performance Lithium–Sulfur Batteries
journal, January 2018


High rate and stable cycling of lithium metal anode
journal, February 2015

  • Qian, Jiangfeng; Henderson, Wesley A.; Xu, Wu
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7362

A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries
journal, February 2013

  • Suo, Liumin; Hu, Yong-Sheng; Li, Hong
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2513

Stable Lithium Electrodeposition at Ultra-High Current Densities Enabled by 3D PMF/Li Composite Anode
journal, February 2018

  • Fan, Lei; Zhuang, Houlong L.; Zhang, Weidong
  • Advanced Energy Materials, Vol. 8, Issue 15
  • DOI: 10.1002/aenm.201703360

Dendrite-Free Lithium Deposition Induced by Uniformly Distributed Lithium Ions for Efficient Lithium Metal Batteries
journal, February 2016

  • Cheng, Xin-Bing; Hou, Ting-Zheng; Zhang, Rui
  • Advanced Materials, Vol. 28, Issue 15
  • DOI: 10.1002/adma.201506124

Polymer Nanofiber-Guided Uniform Lithium Deposition for Battery Electrodes
journal, April 2015

  • Liang, Zheng; Zheng, Guangyuan; Liu, Chong
  • Nano Letters, Vol. 15, Issue 5
  • DOI: 10.1021/nl5046318

Layered reduced graphene oxide with nanoscale interlayer gaps as a stable host for lithium metal anodes
journal, March 2016

  • Lin, Dingchang; Liu, Yayuan; Liang, Zheng
  • Nature Nanotechnology, Vol. 11, Issue 7
  • DOI: 10.1038/nnano.2016.32

Lithium-coated polymeric matrix as a minimum volume-change and dendrite-free lithium metal anode
journal, March 2016

  • Liu, Yayuan; Lin, Dingchang; Liang, Zheng
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10992

Fractal growth of copper electrodeposits
journal, May 1984


Regulation of ramified electrochemical growth by a diffusive wave
journal, August 1995


III. On the concentration at the electrodes in a solution, with special reference to the liberation of hydrogen by electrolysis of a mixture of copper sulphate and sulphuric acid
journal, January 1901

  • Sand, Henry J. S.
  • The London, Edinburgh, and Dublin Philosophical Magazine and Journal of Science, Vol. 1, Issue 1
  • DOI: 10.1080/14786440109462590

Accommodating lithium into 3D current collectors with a submicron skeleton towards long-life lithium metal anodes
journal, August 2015

  • Yang, Chun-Peng; Yin, Ya-Xia; Zhang, Shuai-Feng
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9058

Chemical Dealloying Derived 3D Porous Current Collector for Li Metal Anodes
journal, May 2016


Stable Li Plating/Stripping Electrochemistry Realized by a Hybrid Li Reservoir in Spherical Carbon Granules with 3D Conducting Skeletons
journal, April 2017

  • Ye, Huan; Xin, Sen; Yin, Ya-Xia
  • Journal of the American Chemical Society, Vol. 139, Issue 16
  • DOI: 10.1021/jacs.7b01763

Graphitized Carbon Fibers as Multifunctional 3D Current Collectors for High Areal Capacity Li Anodes
journal, June 2017

  • Zuo, Tong-Tong; Wu, Xiong-Wei; Yang, Chun-Peng
  • Advanced Materials, Vol. 29, Issue 29
  • DOI: 10.1002/adma.201700389

Engineering Flows in Small Devices
journal, January 2004


Nonlinear dynamics of ion concentration polarization in porous media: The leaky membrane model
journal, August 2013

  • Dydek, E. Victoria; Bazant, Martin Z.
  • AIChE Journal, Vol. 59, Issue 9
  • DOI: 10.1002/aic.14200

Overlimiting Current in a Microchannel
journal, September 2011


Measurement and interpretation of electrokinetic phenomena
journal, May 2007

  • Delgado, A. V.; González-Caballero, F.; Hunter, R. J.
  • Journal of Colloid and Interface Science, Vol. 309, Issue 2
  • DOI: 10.1016/j.jcis.2006.12.075

Omniphilic Polymeric Sponges by Ice Templating
journal, February 2016


Soft Colloidal Scaffolds Capable of Elastic Recovery after Large Compressive Strains
journal, August 2014

  • Rajamanickam, Raja; Kumari, Sushma; Kumar, Deepak
  • Chemistry of Materials, Vol. 26, Issue 17
  • DOI: 10.1021/cm502643a

Works referencing / citing this record:

A Game Changer: Functional Nano/Micromaterials for Smart Rechargeable Batteries
journal, August 2019

  • Ryu, Jaegeon; Song, Woo‐Jin; Lee, Sangyeop
  • Advanced Functional Materials, Vol. 30, Issue 2
  • DOI: 10.1002/adfm.201902499

Highly Elastic Polyrotaxane Binders for Mechanically Stable Lithium Hosts in Lithium‐Metal Batteries
journal, May 2019

  • Yoo, Dong‐Joo; Elabd, Ahmed; Choi, Sunghun
  • Advanced Materials, Vol. 31, Issue 29
  • DOI: 10.1002/adma.201901645

Electrokinetic Phenomena Enhanced Lithium‐Ion Transport in Leaky Film for Stable Lithium Metal Anodes
journal, April 2019


Flexible Amalgam Film Enables Stable Lithium Metal Anodes with High Capacities
journal, November 2019

  • He, Guang; Li, Qingwen; Shen, Yongli
  • Angewandte Chemie International Edition, Vol. 58, Issue 51
  • DOI: 10.1002/anie.201911800

Gradient‐Distributed Nucleation Seeds on Conductive Host for a Dendrite‐Free and High‐Rate Lithium Metal Anode
journal, September 2019


Constructing Ionic Gradient and Lithiophilic Interphase for High‐Rate Li‐Metal Anode
journal, October 2019


Conductive carbon nanofiber interpenetrated graphene architecture for ultra-stable sodium ion battery
journal, September 2019


Lithiophilic montmorillonite serves as lithium ion reservoir to facilitate uniform lithium deposition
journal, October 2019


Biomacromolecules enabled dendrite-free lithium metal battery and its origin revealed by cryo-electron microscopy
journal, January 2020


Challenges and opportunities towards fast-charging battery materials
journal, June 2019


Polymer–inorganic solid–electrolyte interphase for stable lithium metal batteries under lean electrolyte conditions
journal, March 2019


Demulsification-induced fast solidification: a novel strategy for the preparation of polymer films
journal, January 2019

  • Wang, Dan; Ge, Xingshi; Nie, Heran
  • Chemical Communications, Vol. 55, Issue 62
  • DOI: 10.1039/c9cc03925b

Facile synthesis of Ti 4 O 7 on hollow carbon spheres with enhanced polysulfide binding for high-performance lithium–sulfur batteries
journal, January 2019

  • Wang, Fang; Ding, Xian; Shi, Ruyue
  • Journal of Materials Chemistry A, Vol. 7, Issue 17
  • DOI: 10.1039/c9ta00544g

Mitigating concentration polarization for highly reversible plating/stripping electrochemistry: Li versus Na
journal, January 2019

  • Tang, Shuai; Zhang, Xia-Guang; Cui, Xue-Yang
  • Journal of Materials Chemistry A, Vol. 7, Issue 40
  • DOI: 10.1039/c9ta08312j

Stable and Safe Lithium Metal Batteries with Ni-Rich Cathodes Enabled by a High Efficiency Flame Retardant Additive
journal, January 2019

  • Li, Yuan; An, Yongling; Tian, Yuan
  • Journal of The Electrochemical Society, Vol. 166, Issue 13
  • DOI: 10.1149/2.0081913jes

A Sponge-Driven Elastic Interface for Lithium Metal Anodes
journal, September 2019


Lithiophilic montmorillonite serves as lithium ion reservoir to facilitate uniform lithium deposition
journal, October 2019


A Sponge-Driven Elastic Interface for Lithium Metal Anodes
journal, September 2019