skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Fabrication of Low-Tortuosity Ultrahigh-Area-Capacity Battery Electrodes through Magnetic Alignment of Emulsion-Based Slurries

Abstract

High energy–density, low–cost batteries are critically important to a variety of applications ranging from portable electronics to electric vehicles (EVs) and grid–scale storage. While tremendous research effort has been focused on new materials or chemistries with high energy–density potential, design innovations such as low–tortuosity thick electrodes are another promising path toward higher energy density and lower cost. Growing demand for fast–charging batteries has also highlighted the need for negative electrodes that can accept high rate charging without metal deposition; low tortuosity can be a benefit in this regard. However, a general and scalable fabrication method for low–tortuosity electrodes is currently lacking. Here an emulsion–based, magnetic–alignment approach to producing thick electrodes (>400 µm thickness) with ultrahigh areal capacity (up to ≈14 mAh cm–2 vs 2–4 mAh cm–2 for conventional lithium ion) is reported. The process is demonstrated for LiCoO2 and meso–carbon microbead graphite. The LiCoO2 cathodes are confirmed to have low tortuosity via DC–depolarization experiments and deliver high areal capacity (>10 mAh cm–2) in galvanostatic discharge tests at practical C–rates and model EV drive–cycle tests. Lastly, this simple fabrication method can potentially be applied to many other active materials to enable thick, low–tortuosity electrodes.

Authors:
 [1];  [2];  [3];  [3]; ORCiD logo [4]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Shanghai Jiao Tong Univ., Shanghai, (China); Shanghai Electrochemical Energy Devices Research Center, Shanghai (China)
  2. Northeastern Univ., Boston, MA (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1498274
Alternate Identifier(s):
OSTI ID: 1483709
Report Number(s):
BNL-211313-2019-JAAM
Journal ID: ISSN 1614-6832
Grant/Contract Number:  
SC0012704; AC02-05CH11231; 7056592; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 2; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; emulsion; low‐tortuosity; magnetic alignment; thick electrodes

Citation Formats

Li, Linsen, Erb, Randall M., Wang, Jiajun, Wang, Jun, and Chiang, Yet -Ming. Fabrication of Low-Tortuosity Ultrahigh-Area-Capacity Battery Electrodes through Magnetic Alignment of Emulsion-Based Slurries. United States: N. p., 2018. Web. doi:10.1002/aenm.201802472.
Li, Linsen, Erb, Randall M., Wang, Jiajun, Wang, Jun, & Chiang, Yet -Ming. Fabrication of Low-Tortuosity Ultrahigh-Area-Capacity Battery Electrodes through Magnetic Alignment of Emulsion-Based Slurries. United States. doi:10.1002/aenm.201802472.
Li, Linsen, Erb, Randall M., Wang, Jiajun, Wang, Jun, and Chiang, Yet -Ming. Wed . "Fabrication of Low-Tortuosity Ultrahigh-Area-Capacity Battery Electrodes through Magnetic Alignment of Emulsion-Based Slurries". United States. doi:10.1002/aenm.201802472. https://www.osti.gov/servlets/purl/1498274.
@article{osti_1498274,
title = {Fabrication of Low-Tortuosity Ultrahigh-Area-Capacity Battery Electrodes through Magnetic Alignment of Emulsion-Based Slurries},
author = {Li, Linsen and Erb, Randall M. and Wang, Jiajun and Wang, Jun and Chiang, Yet -Ming},
abstractNote = {High energy–density, low–cost batteries are critically important to a variety of applications ranging from portable electronics to electric vehicles (EVs) and grid–scale storage. While tremendous research effort has been focused on new materials or chemistries with high energy–density potential, design innovations such as low–tortuosity thick electrodes are another promising path toward higher energy density and lower cost. Growing demand for fast–charging batteries has also highlighted the need for negative electrodes that can accept high rate charging without metal deposition; low tortuosity can be a benefit in this regard. However, a general and scalable fabrication method for low–tortuosity electrodes is currently lacking. Here an emulsion–based, magnetic–alignment approach to producing thick electrodes (>400 µm thickness) with ultrahigh areal capacity (up to ≈14 mAh cm–2 vs 2–4 mAh cm–2 for conventional lithium ion) is reported. The process is demonstrated for LiCoO2 and meso–carbon microbead graphite. The LiCoO2 cathodes are confirmed to have low tortuosity via DC–depolarization experiments and deliver high areal capacity (>10 mAh cm–2) in galvanostatic discharge tests at practical C–rates and model EV drive–cycle tests. Lastly, this simple fabrication method can potentially be applied to many other active materials to enable thick, low–tortuosity electrodes.},
doi = {10.1002/aenm.201802472},
journal = {Advanced Energy Materials},
number = 2,
volume = 9,
place = {United States},
year = {2018},
month = {11}
}

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

Citation Metrics:
Cited by: 9 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

How the electrolyte limits fast discharge in nanostructured batteries and supercapacitors
journal, November 2009

  • Johns, Phil A.; Roberts, Matthew R.; Wakizaka, Yasuaki
  • Electrochemistry Communications, Vol. 11, Issue 11
  • DOI: 10.1016/j.elecom.2009.09.001

Direct Measurements of Effective Ionic Transport in Porous Li-Ion Electrodes
journal, December 2012

  • Zacharias, Nathan A.; Nevers, Douglas R.; Skelton, Cole
  • Journal of The Electrochemical Society, Vol. 160, Issue 2
  • DOI: 10.1149/2.062302jes

Building better batteries
journal, February 2008

  • Armand, M.; Tarascon, J.-M.
  • Nature, Vol. 451, Issue 7179, p. 652-657
  • DOI: 10.1038/451652a

Ultrahigh-Energy-Density Microbatteries Enabled by New Electrode Architecture and Micropackaging Design
journal, May 2010

  • Lai, Wei; Erdonmez, Can K.; Marinis, Thomas F.
  • Advanced Materials, Vol. 22, Issue 20
  • DOI: 10.1002/adma.200903650

Carbon-Encapsulated Fe 3 O 4 Nanoparticles as a High-Rate Lithium Ion Battery Anode Material
journal, April 2013

  • He, Chunnian; Wu, Shan; Zhao, Naiqin
  • ACS Nano, Vol. 7, Issue 5
  • DOI: 10.1021/nn401059h

Lithium Batteries and Cathode Materials
journal, October 2004

  • Whittingham, M. Stanley
  • Chemical Reviews, Vol. 104, Issue 10, p. 4271-4302
  • DOI: 10.1021/cr020731c

Magnetically aligned graphite electrodes for high-rate performance Li-ion batteries
journal, July 2016

  • Billaud, Juliette; Bouville, Florian; Magrini, Tommaso
  • Nature Energy, Vol. 1, Issue 8
  • DOI: 10.1038/nenergy.2016.97

Review—Li-Rich Layered Oxide Cathodes for Next-Generation Li-Ion Batteries: Chances and Challenges
journal, January 2015

  • Rozier, Patrick; Tarascon, Jean Marie
  • Journal of The Electrochemical Society, Vol. 162, Issue 14
  • DOI: 10.1149/2.0111514jes

High-performance battery electrodes via magnetic templating
journal, July 2016


Local Tortuosity Inhomogeneities in a Lithium Battery Composite Electrode
journal, January 2011

  • Kehrwald, Dirk; Shearing, Paul R.; Brandon, Nigel P.
  • Journal of The Electrochemical Society, Vol. 158, Issue 12
  • DOI: 10.1149/2.079112jes

Li–O2 and Li–S batteries with high energy storage
journal, January 2012

  • Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J.
  • Nature Materials, Vol. 11, Issue 1, p. 19-29
  • DOI: 10.1038/nmat3191

Design of Battery Electrodes with Dual-Scale Porosity to Minimize Tortuosity and Maximize Performance
journal, December 2012

  • Bae, Chang-Jun; Erdonmez, Can K.; Halloran, John W.
  • Advanced Materials, Vol. 25, Issue 9
  • DOI: 10.1002/adma.201204055

Nickel-Rich and Lithium-Rich Layered Oxide Cathodes: Progress and Perspectives
journal, October 2015

  • Manthiram, Arumugam; Knight, James C.; Myung, Seung-Taek
  • Advanced Energy Materials, Vol. 6, Issue 1
  • DOI: 10.1002/aenm.201501010

Cost modeling of lithium-ion battery cells for automotive applications
journal, October 2014

  • Patry, Gaëtan; Romagny, Alex; Martinet, Sébastien
  • Energy Science & Engineering, Vol. 3, Issue 1
  • DOI: 10.1002/ese3.47

Optimizing Areal Capacities through Understanding the Limitations of Lithium-Ion Electrodes
journal, November 2015

  • Gallagher, Kevin G.; Trask, Stephen E.; Bauer, Christoph
  • Journal of The Electrochemical Society, Vol. 163, Issue 2
  • DOI: 10.1149/2.0321602jes

Quantifying tortuosity in porous Li-ion battery materials
journal, March 2009