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

Handle URI:
http://hdl.handle.net/10754/597226
Title:
A Catalytic Path for Electrolyte Reduction in Lithium-Ion Cells Revealed by in Situ Attenuated Total Reflection-Fourier Transform Infrared Spectroscopy
Authors:
Shi, Feifei; Ross, Philip N.; Zhao, Hui; Liu, Gao; Somorjai, Gabor A.; Komvopoulos, Kyriakos
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.
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
Issue Date:
11-Mar-2015
DOI:
10.1021/ja5128456
PubMed ID:
25689135
Type:
Article
ISSN:
0002-7863; 1520-5126
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.
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Full metadata record

DC FieldValue Language
dc.contributor.authorShi, Feifeien
dc.contributor.authorRoss, Philip N.en
dc.contributor.authorZhao, Huien
dc.contributor.authorLiu, Gaoen
dc.contributor.authorSomorjai, Gabor A.en
dc.contributor.authorKomvopoulos, Kyriakosen
dc.date.accessioned2016-02-25T12:28:23Zen
dc.date.available2016-02-25T12:28:23Zen
dc.date.issued2015-03-11en
dc.identifier.citationShi 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.en
dc.identifier.issn0002-7863en
dc.identifier.issn1520-5126en
dc.identifier.pmid25689135en
dc.identifier.doi10.1021/ja5128456en
dc.identifier.urihttp://hdl.handle.net/10754/597226en
dc.description.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.en
dc.description.sponsorshipThis 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.en
dc.publisherAmerican Chemical Society (ACS)en
dc.titleA Catalytic Path for Electrolyte Reduction in Lithium-Ion Cells Revealed by in Situ Attenuated Total Reflection-Fourier Transform Infrared Spectroscopyen
dc.typeArticleen
dc.identifier.journalJournal of the American Chemical Societyen
dc.contributor.institutionUC Berkeley, Berkeley, United Statesen
dc.contributor.institutionLawrence Berkeley National Laboratory, Berkeley, United Statesen
kaust.grant.programAcademic Excellence Alliance (AEA)en
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