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Title: Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries

Authors:
 [1];  [2];  [2];  [2]; ORCiD logo [1]
  1. The Joint Center for Energy Storage Research (JCESR), Pacific Northwest National Laboratory, Richland WA 99354 USA, Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland WA 99354 USA
  2. Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland WA 99354 USA
Publication Date:
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1399051
Grant/Contract Number:
AC02-05CH11231
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Related Information: CHORUS Timestamp: 2017-10-11 08:06:53; Journal ID: ISSN 1614-6832
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Adams, Brian D., Zheng, Jianming, Ren, Xiaodi, Xu, Wu, and Zhang, Ji-Guang. Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries. Germany: N. p., 2017. Web. doi:10.1002/aenm.201702097.
Adams, Brian D., Zheng, Jianming, Ren, Xiaodi, Xu, Wu, & Zhang, Ji-Guang. Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries. Germany. doi:10.1002/aenm.201702097.
Adams, Brian D., Zheng, Jianming, Ren, Xiaodi, Xu, Wu, and Zhang, Ji-Guang. 2017. "Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries". Germany. doi:10.1002/aenm.201702097.
@article{osti_1399051,
title = {Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries},
author = {Adams, Brian D. and Zheng, Jianming and Ren, Xiaodi and Xu, Wu and Zhang, Ji-Guang},
abstractNote = {},
doi = {10.1002/aenm.201702097},
journal = {Advanced Energy Materials},
number = ,
volume = ,
place = {Germany},
year = 2017,
month =
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on October 11, 2018
Publisher's Accepted Manuscript

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  • We report that lithium (Li) metal batteries (LMBs) have recently attracted extensive interest in the energy-storage field after silence from the public view for several decades. However, many challenges still need to be overcome before their practical application, especially those that are related to the interfacial instability of Li metal anodes. Here, we reveal for the first time that the thickness of the degradation layer on the metallic Li anode surface shows a linear relationship with Li areal capacity utilization up to 4.0 mAh cm -2 in a practical LMB system. The increase in Li capacity utilization in each cyclemore » causes variations in the morphology and composition of the degradation layer on the Li anode. Under high Li capacity utilization, the current density for charge (i.e., Li deposition) is identified to be a key factor controlling the corrosion of the Li metal anode. Lastly, these fundamental findings provide new perspectives for the development of rechargeable LMBs.« less
  • Lithium (Li) metal batteries (LMBs) are regarded as the most promising power sources for electric vehicles. Besides the Li dendrite growth and low Li Coulombic efficiency, how to well match Li metal anode with a high loading (normally over 3.0 mAh cm-2) cathode is another key challenge to achieve the real high energy density battery. In this work, we systematically investigate the effects of the Li metal capacity usage in each cycle, manipulated by varying the cathode areal loading, on the stability of Li metal anode and the cycling performance of LMBs using the LiNi1/3Mn1/3Co1/3O2 (NMC) cathode and an additive-containingmore » dual-salt/carbonate-solvent electrolyte. It is demonstrated that the Li||NMC cells show decent long-term cycling performance even with NMC areal capacity loading up to ca. 4.0 mAh cm-2 and at a charge current density of 1.0 mA cm-2. The increase of the Li capacity usage in each cycle causes variation in the components of the solid electrolyte interphase (SEI) layer on Li metal anode and generates more ionic conductive species from this electrolyte. Further study reveals for the first time that the degradation of Li metal anode and the thickness of SEI layer on Li anode show linear relationship with the areal capacity of NMC cathode. Meanwhile, the expansion rate of consumed Li and the ratio of SEI thickness to NMC areal loading are kept almost the same value with increasing cathode loading, respectively. These fundamental findings provide new perspectives on the rational evaluation of Li metal anode stability for the development of rechargeable LMBs.« less
  • Rechargeable lithium metal batteries have much higher energy density than those of lithium ion batteries using graphite anode. Unfortunately, uncontrollable dendritic lithium growth inherent in these batteries (upon repeated charge/discharge cycling) and limited Coulombic efficiency during lithium deposition/striping has prevented their practical application over the past 40 years. With the emerging of post Li-ion batteries, safe and efficient operation of lithium metal anode has become an enabling technology which may determine the fate of several promising candidates for the next generation of energy storage systems, including rechargeable Li-air battery, Li-S battery, and Li metal battery which utilize lithium intercalation compoundsmore » as cathode. In this work, various factors which affect the morphology and Coulombic efficiency of lithium anode will be analyzed. Technologies used to characterize the morphology of lithium deposition and the results obtained by modeling of lithium dendrite growth will also be reviewed. At last, recent development in this filed and urgent need in this field will also be discussed.« less
  • With the significant progress made in the development of cathodes in lithium-sulfur (Li-S) batteries, the stability of Li metal anodes becomes a more urgent challenge in these batteries. Here we report the systematic investigation of the stability of the anode/electrolyte interface in Li-S batteries with concentrated electrolytes containing various lithium salts. It is found that Li-S batteries using LiTFSI-based electrolytes are more stable than those using LiFSI-based electrolytes. The decreased stability is because the N-S bond in the FSI- anion is fairly weak and the scission of this bond leads to the formation of lithium sulfate (LiSOx) in the presencemore » of polysulfide species. In contrast, even the weakest bond (C-S) in the TFSI- anion is stronger than the N-S bond in the FSI- anion. In the LiTFSI-based electrolyte, the lithium metal anode tends to react with polysulfide to form lithium sulfide (LiSx) which is more reversible than LiSOx formed in the LiTFSI-based electrolyte. This fundamental difference in the bond strength of the salt anions in the presence of polysulfide species leads to a large difference in the stability of the anode-electrolyte interface and performance of the Li-S batteries with electrolytes composed of these salts. Therefore, anion selection is one of the key parameters in the search for new electrolytes for stable operation of Li-S batteries.« less