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    A Catalytic Path for Electrolyte Reduction in Lithium-Ion Cells Revealed by in Situ Attenuated Total Reflection-Fourier Transform Infrared Spectroscopy

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    Type
    Article
    Authors
    Shi, Feifei
    Ross, Philip N.
    Zhao, Hui
    Liu, Gao
    Somorjai, Gabor A.
    Komvopoulos, Kyriakos
    Date
    2015-02-25
    Online Publication Date
    2015-02-25
    Print Publication Date
    2015-03-11
    Permanent link to this record
    http://hdl.handle.net/10754/597226
    
    Metadata
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    Abstract
    © 2015 American Chemical Society. Although controlling the interfacial chemistry of electrodes in Li-ion batteries (LIBs) is crucial for maintaining the reversibility, electrolyte decomposition has not been fully understood. In this study, electrolyte decomposition on model electrode surfaces (Au and Sn) was investigated by in situ attenuated total reflection-Fourier transform infrared (ATR-FTIR) spectroscopy. Simultaneously obtained ATR-FTIR spectra and cyclic voltammetry measurements show that lithium ethylene dicarbonate and lithium propionate form on the Au electrode at 0.6 V, whereas diethyl 2,5-dioxahexane dicarboxylate and lithium propionate form on the Sn electrode surface at 1.25 V. A noncatalytic reduction path on the Au surface and a catalytic reduction path on the Sn surface are introduced to explain the surface dependence of the overpotential and product selectivity. This represents a new concept for explaining electrolyte reactions on the anode of LIBs. The present investigation shows that catalysis plays a dominant role in the electrolyte decomposition process and has important implications in electrode surface modification and electrolyte recipe selection, which are critical factors for enhancing the efficiency, durability, and reliability of LIBs.
    Citation
    Shi F, Ross PN, Zhao H, Liu G, Somorjai GA, et al. (2015) A Catalytic Path for Electrolyte Reduction in Lithium-Ion Cells Revealed by in Situ Attenuated Total Reflection-Fourier Transform Infrared Spectroscopy . Journal of the American Chemical Society 137: 3181–3184. Available: http://dx.doi.org/10.1021/ja5128456.
    Sponsors
    This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Freedom CAR and Vehicle Technologies of the U.S. Department of Energy under Contract No. DE-AC02 O5CH1123. The last author (K.K.) also acknowledges the funding provided for this work by the UCB-KAUST Academic Excellence Alliance (AEA) Program. The IR instrumentation was purchased with funding from the Director, Office of Basic Energy Sciences, Materials Science and Engineering Division of the U.S, Department of Energy.
    Publisher
    American Chemical Society (ACS)
    Journal
    Journal of the American Chemical Society
    DOI
    10.1021/ja5128456
    PubMed ID
    25689135
    ae974a485f413a2113503eed53cd6c53
    10.1021/ja5128456
    Scopus Count
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