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

Title: Understanding the critical chemistry to inhibit lithium consumption in lean lithium metal composite anodes

Abstract

Lithium metal has been deemed by many as the “Holy Grail” of anode materials due to its high theoretical capacity (~3860 mA h g-1), redox potential of -3.040 V vs. SHE, and light weight. The goal of this work is to investigate the relationship between a lean lithium metal anode and its consumption as a function of host materials, electrochemical protocol and electrolyte composition. With the use of carbon nanofibers, lithium metal has been electrodeposited onto the host matrix and used in a battery with a LiNi0.6Mn0.2Co0.2O2 cathode. The mass-loading of lithium can be easily controlled and utilized to investigate the practicality of an anode limited battery (i.e., limited lithium with an effective thickness <15 μm) in a high surface area matrix. We then quantify the consumption rate of active lithium using different electrolyte additives and current rates in full cells and observe that the lithium consumption behavior in an anode-limited cell is different from that in an anode-excess cell. Our results highlight the necessity of applying truly lithium-limited cells when evaluating the electrochemical properties of lithium anodes and electrolyte additives. By extending this method to a standard graphite host, full cells can retain 75% of their initial capacities aftermore » 1000 cycles. The present study demonstrates the importance of graphitic carbon in increasing the lifespan of limited lithium (<15 μm) for practical lithium metal batteries.« less

Authors:
 [1]; ORCiD logo [2];  [1];  [3];  [1]; ORCiD logo [4]; ORCiD logo [1]
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Chemistry
  2. Southwest Forestry Univ., Kunming (China). National Joint Engineering Research Center for Highly-Efficient Utilization Technology of Forest Biomass Resources and College of Materials Science and Engineering
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  4. Southwest Forestry Univ., Kunming (China). National Joint Engineering Research Center for Highly-Efficient Utilization Technology of Forest Biomass Resources and College of Materials Science and Engineering; Xiamen Univ. (China). College of Energy and Fujian Engineering and Research Center of Clean and High-Valued Technologies for Biomass
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1476323
Grant/Contract Number:  
AC02-76SF00515; 31160147; 2014FA034; 2017YFD0601003
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 6; Journal Issue: 33; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 25 ENERGY STORAGE

Citation Formats

Kautz, David J., Tao, Lei, Mu, Linqin, Nordlund, Dennis, Feng, Xu, Zheng, Zhifeng, and Lin, Feng. Understanding the critical chemistry to inhibit lithium consumption in lean lithium metal composite anodes. United States: N. p., 2018. Web. doi:10.1039/c8ta01715h.
Kautz, David J., Tao, Lei, Mu, Linqin, Nordlund, Dennis, Feng, Xu, Zheng, Zhifeng, & Lin, Feng. Understanding the critical chemistry to inhibit lithium consumption in lean lithium metal composite anodes. United States. https://doi.org/10.1039/c8ta01715h
Kautz, David J., Tao, Lei, Mu, Linqin, Nordlund, Dennis, Feng, Xu, Zheng, Zhifeng, and Lin, Feng. Tue . "Understanding the critical chemistry to inhibit lithium consumption in lean lithium metal composite anodes". United States. https://doi.org/10.1039/c8ta01715h. https://www.osti.gov/servlets/purl/1476323.
@article{osti_1476323,
title = {Understanding the critical chemistry to inhibit lithium consumption in lean lithium metal composite anodes},
author = {Kautz, David J. and Tao, Lei and Mu, Linqin and Nordlund, Dennis and Feng, Xu and Zheng, Zhifeng and Lin, Feng},
abstractNote = {Lithium metal has been deemed by many as the “Holy Grail” of anode materials due to its high theoretical capacity (~3860 mA h g-1), redox potential of -3.040 V vs. SHE, and light weight. The goal of this work is to investigate the relationship between a lean lithium metal anode and its consumption as a function of host materials, electrochemical protocol and electrolyte composition. With the use of carbon nanofibers, lithium metal has been electrodeposited onto the host matrix and used in a battery with a LiNi0.6Mn0.2Co0.2O2 cathode. The mass-loading of lithium can be easily controlled and utilized to investigate the practicality of an anode limited battery (i.e., limited lithium with an effective thickness <15 μm) in a high surface area matrix. We then quantify the consumption rate of active lithium using different electrolyte additives and current rates in full cells and observe that the lithium consumption behavior in an anode-limited cell is different from that in an anode-excess cell. Our results highlight the necessity of applying truly lithium-limited cells when evaluating the electrochemical properties of lithium anodes and electrolyte additives. By extending this method to a standard graphite host, full cells can retain 75% of their initial capacities after 1000 cycles. The present study demonstrates the importance of graphitic carbon in increasing the lifespan of limited lithium (<15 μm) for practical lithium metal batteries.},
doi = {10.1039/c8ta01715h},
journal = {Journal of Materials Chemistry. A},
number = 33,
volume = 6,
place = {United States},
year = {2018},
month = {7}
}

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

Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: Characterization of the pristine CNF: (a) SEM image of the pristine CNF porous matrix structure, (b) Raman spectrum of the pristine CNF, (c) FTIR spectrum of the pristine CNF, (d and e) TEM images of the pristine CNF at two different magnifications , and (f) electron diffraction patternmore » of the pristine CNF showing the amorphous characteristics of the CNF.« less

Save / Share:

Works referenced in this record:

Mechanical Surface Modification of Lithium Metal: Towards Improved Li Metal Anode Performance by Directed Li Plating
journal, December 2014

  • Ryou, Myung-Hyun; Lee, Yong Min; Lee, Yunju
  • Advanced Functional Materials, Vol. 25, Issue 6
  • DOI: 10.1002/adfm.201402953

All-Integrated Bifunctional Separator for Li Dendrite Detection via Novel Solution Synthesis of a Thermostable Polyimide Separator
journal, August 2016

  • Lin, Dingchang; Zhuo, Denys; Liu, Yayuan
  • Journal of the American Chemical Society, Vol. 138, Issue 34
  • DOI: 10.1021/jacs.6b06324

The synergetic effect of lithium polysulfide and lithium nitrate to prevent lithium dendrite growth
journal, June 2015

  • Li, Weiyang; Yao, Hongbin; Yan, Kai
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8436

Accurate Consumption Analysis of Vinylene Carbonate as an Electrolyte Additive in an 18650 Lithium-Ion Battery at the First Charge-Discharge Cycle
journal, December 2016

  • Haruna, Hiroshi; Takahashi, Shin; Tanaka, Yasutaka
  • Journal of The Electrochemical Society, Vol. 164, Issue 1
  • DOI: 10.1149/2.0441701jes

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


Application of Stabilized Lithium Metal Powder (SLMP®) in graphite anode – A high efficient prelithiation method for lithium-ion batteries
journal, August 2014


Compatibility issues between electrodes and electrolytes in solid-state batteries
journal, January 2017

  • Tian, Yaosen; Shi, Tan; Richards, William D.
  • Energy & Environmental Science, Vol. 10, Issue 5
  • DOI: 10.1039/C7EE00534B

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

Surface reconstruction and chemical evolution of stoichiometric layered cathode materials for lithium-ion batteries
journal, March 2014

  • Lin, Feng; Markus, Isaac M.; Nordlund, Dennis
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4529

Effect of vinylene carbonate as additive to electrolyte for lithium metal anode
journal, February 2004


Effects of Carbonate Solvents and Lithium Salts on Morphology and Coulombic Efficiency of Lithium Electrode
journal, January 2013

  • Ding, Fei; Xu, Wu; Chen, Xilin
  • Journal of The Electrochemical Society, Vol. 160, Issue 10
  • DOI: 10.1149/2.100310jes

An Artificial Solid Electrolyte Interphase Layer for Stable Lithium Metal Anodes
journal, December 2015


Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal
journal, January 2017


How dynamic is the SEI?
journal, December 2007


High-Energy All-Solid-State Lithium Batteries with Ultralong Cycle Life
journal, October 2016


Reviving the lithium metal anode for high-energy batteries
journal, March 2017

  • Lin, Dingchang; Liu, Yayuan; Cui, Yi
  • Nature Nanotechnology, Vol. 12, Issue 3
  • DOI: 10.1038/nnano.2017.16

Composite lithium metal anode by melt infusion of lithium into a 3D conducting scaffold with lithiophilic coating
journal, February 2016

  • Liang, Zheng; Lin, Dingchang; Zhao, Jie
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 11
  • DOI: 10.1073/pnas.1518188113

Implantable Solid Electrolyte Interphase in Lithium-Metal Batteries
journal, February 2017


Corrosion/Fragmentation of Layered Composite Cathode and Related Capacity/Voltage Fading during Cycling Process
journal, July 2013

  • Zheng, Jianming; Gu, Meng; Xiao, Jie
  • Nano Letters, Vol. 13, Issue 8
  • DOI: 10.1021/nl401849t

Micromorphological Studies of Lithium Electrodes in Alkyl Carbonate Solutions Using in Situ Atomic Force Microscopy
journal, December 2000

  • Cohen, Yaron S.; Cohen, Yair; Aurbach, Doron
  • The Journal of Physical Chemistry B, Vol. 104, Issue 51
  • DOI: 10.1021/jp002526b

Making Li-metal electrodes rechargeable by controlling the dendrite growth direction
journal, June 2017


Understanding the Degradation Mechanisms of LiNi 0.5 Co 0.2 Mn 0.3 O 2 Cathode Material in Lithium Ion Batteries
journal, August 2013

  • Jung, Sung-Kyun; Gwon, Hyeokjo; Hong, Jihyun
  • Advanced Energy Materials, Vol. 4, Issue 1
  • DOI: 10.1002/aenm.201300787

Nanoscale Morphological and Chemical Changes of High Voltage Lithium–Manganese Rich NMC Composite Cathodes with Cycling
journal, July 2014

  • Yang, Feifei; Liu, Yijin; Martha, Surendra K.
  • Nano Letters, Vol. 14, Issue 8
  • DOI: 10.1021/nl502090z

Very Stable Lithium Metal Stripping–Plating at a High Rate and High Areal Capacity in Fluoroethylene Carbonate-Based Organic Electrolyte Solution
journal, May 2017


Free-Standing Hollow Carbon Fibers as High-Capacity Containers for Stable Lithium Metal Anodes
journal, November 2017


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


Interface Stability in Solid-State Batteries
journal, December 2015


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

Fluoroethylene Carbonate and Vinylene Carbonate Reduction: Understanding Lithium-Ion Battery Electrolyte Additives and Solid Electrolyte Interphase Formation
journal, November 2016


A review of lithium deposition in lithium-ion and lithium metal secondary batteries
journal, May 2014


Solution-Processable Glass LiI-Li 4 SnS 4 Superionic Conductors for All-Solid-State Li-Ion Batteries
journal, December 2015

  • Park, Kern Ho; Oh, Dae Yang; Choi, Young Eun
  • Advanced Materials, Vol. 28, Issue 9
  • DOI: 10.1002/adma.201505008

Thermal and Rheological Characteristics of Biobased Carbon Fiber Precursor Derived from Low Molecular Weight Organosolv Lignin
journal, March 2015


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

Status and challenges in enabling the lithium metal electrode for high-energy and low-cost rechargeable batteries
journal, December 2017


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

First Evidence of Manganese–Nickel Segregation and Densification upon Cycling in Li-Rich Layered Oxides for Lithium Batteries
journal, July 2013

  • Boulineau, Adrien; Simonin, Loïc; Colin, Jean-François
  • Nano Letters, Vol. 13, Issue 8
  • DOI: 10.1021/nl4019275

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

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


Fluoroethylene Carbonate and Vinylene Carbonate Reduction: Understanding Lithium-Ion Battery Electrolyte Additives and Solid Electrolyte Interphase Formation
text, January 2016

  • Michan, Alison; Parimalam, Bs; Leskes, Michal
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.6951

Works referencing / citing this record:

High‐Voltage Charging‐Induced Strain, Heterogeneity, and Micro‐Cracks in Secondary Particles of a Nickel‐Rich Layered Cathode Material
journal, March 2019

  • Mao, Yuwei; Wang, Xuelong; Xia, Sihao
  • Advanced Functional Materials, Vol. 29, Issue 18
  • DOI: 10.1002/adfm.201900247

Correlation between Li Plating Behavior and Surface Characteristics of Carbon Matrix toward Stable Li Metal Anodes
journal, November 2018

  • Cui, Jiang; Yao, Shanshan; Ihsan-Ul-Haq, Muhammad
  • Advanced Energy Materials, Vol. 9, Issue 1
  • DOI: 10.1002/aenm.201802777

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.