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Title: Redox probing study of the potential dependence of charge transport through Li2O2

Abstract

In the field of energy storage devices the pursuit for cheap, high energy density, reliable secondary batteries is at the top of the agenda. The Li–O2 battery is one of the possible technologies that, in theory, should be able to close the gap, which exists between the present state-of-the-art Li-ion technologies and the demand placed on batteries by technologies such as electrical vehicles. Here we present a redox probing study of the charge transfer across the main deposition product lithium peroxide, Li2O2, in the Li–O2 battery using outer-sphere redox shuttles. The change in heterogeneous electron transfer exchange rate as a function of the potential and the Li2O2 layer thickness (~depth-of-discharge) was determined using electrochemical impedance spectroscopy. In addition, the attenuation of the electron transfer exchange rate with film thickness is dependent on the probing potential, providing evidence that hole transport is the dominant process for charge transfer through Li2O2 and showing that the origin of the sudden death observed upon discharge is due to charge transport limitations.

Authors:
 [1];  [2];  [1];  [1];  [1]
+ Show Author Affiliations
  1. Technical Univ. of Denmark, Roskilde (Denmark)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1230058
Grant/Contract Number:  
11-116792; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 119; Journal Issue: C; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Knudsen, Kristian B., Luntz, Alan C., Jensen, Søren H., Vegge, Tejs, and Hjelm, Johan. Redox probing study of the potential dependence of charge transport through Li2O2. United States: N. p., 2015. Web. doi:10.1021/acs.jpcc.5b08757.
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Knudsen, Kristian B., Luntz, Alan C., Jensen, Søren H., Vegge, Tejs, & Hjelm, Johan. Redox probing study of the potential dependence of charge transport through Li2O2. United States. https://doi.org/10.1021/acs.jpcc.5b08757
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Knudsen, Kristian B., Luntz, Alan C., Jensen, Søren H., Vegge, Tejs, and Hjelm, Johan. Fri . "Redox probing study of the potential dependence of charge transport through Li2O2". United States. https://doi.org/10.1021/acs.jpcc.5b08757. https://www.osti.gov/servlets/purl/1230058.
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@article{osti_1230058,
title = {Redox probing study of the potential dependence of charge transport through Li2O2},
author = {Knudsen, Kristian B. and Luntz, Alan C. and Jensen, Søren H. and Vegge, Tejs and Hjelm, Johan},
abstractNote = {In the field of energy storage devices the pursuit for cheap, high energy density, reliable secondary batteries is at the top of the agenda. The Li–O2 battery is one of the possible technologies that, in theory, should be able to close the gap, which exists between the present state-of-the-art Li-ion technologies and the demand placed on batteries by technologies such as electrical vehicles. Here we present a redox probing study of the charge transfer across the main deposition product lithium peroxide, Li2O2, in the Li–O2 battery using outer-sphere redox shuttles. The change in heterogeneous electron transfer exchange rate as a function of the potential and the Li2O2 layer thickness (~depth-of-discharge) was determined using electrochemical impedance spectroscopy. In addition, the attenuation of the electron transfer exchange rate with film thickness is dependent on the probing potential, providing evidence that hole transport is the dominant process for charge transfer through Li2O2 and showing that the origin of the sudden death observed upon discharge is due to charge transport limitations.},
doi = {10.1021/acs.jpcc.5b08757},
journal = {Journal of Physical Chemistry. C},
number = C,
volume = 119,
place = {United States},
year = {Fri Nov 20 00:00:00 EST 2015},
month = {Fri Nov 20 00:00:00 EST 2015}
}
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https://doi.org/10.1021/acs.jpcc.5b08757
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    Works referencing / citing this record:

    Understanding the Reaction Interface in Lithium-Oxygen Batteries
    journal, October 2018

    Amorphous Li 2 O 2 : Chemical Synthesis and Electrochemical Properties
    journal, August 2016

    • Zhang, Yelong; Cui, Qinghua; Zhang, Xinmin
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    • DOI: 10.1002/anie.201605228

    Anomalous Discharge Behavior of Graphite Nanosheet Electrodes in Lithium-Oxygen Batteries
    journal, December 2019

    • Wunderlich, Philipp; Küpper, Jannis; Simon, Ulrich
    • Materials, Vol. 13, Issue 1
    • DOI: 10.3390/ma13010043

    Identifying Reactive Sites and Transport Limitations of Oxygen Reactions in Aprotic Lithium-O 2 Batteries at the Stage of Sudden Death
    journal, March 2016

    • Wang, Jiawei; Zhang, Yelong; Guo, Limin
    • Angewandte Chemie International Edition, Vol. 55, Issue 17
    • DOI: 10.1002/anie.201600793

    Identifying Reactive Sites and Transport Limitations of Oxygen Reactions in Aprotic Lithium-O 2 Batteries at the Stage of Sudden Death
    journal, March 2016

    Understanding the Reaction Interface in Lithium-Oxygen Batteries
    journal, January 2019

    Anomalous Discharge Behavior of Graphite Nanosheet Electrodes in Lithium-Oxygen Batteries
    journal, December 2019

    • Wunderlich, Philipp; Küpper, Jannis; Simon, Ulrich
    • Materials, Vol. 13, Issue 1
    • DOI: 10.3390/ma13010043
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