A catalytic path for electrolyte reduction in lithium-ion cells revealed by in situ attenuated total reflection-fourier transform infrared spectroscopy

Feifei Shi, Philip N. Ross, Hui Zhao, Gao Liu, Gabor A. Somorjai, Kyriakos Komvopoulos

Research output: Contribution to journalArticle

29 Citations (Scopus)

Abstract

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.

Original languageEnglish (US)
Pages (from-to)3181-3184
Number of pages4
JournalJournal of the American Chemical Society
Volume137
Issue number9
DOIs
StatePublished - Feb 2015

Fingerprint

Fourier Transform Infrared Spectroscopy
Lithium
Electrolytes
Fourier transform infrared spectroscopy
Electrodes
Ions
Propionates
Decomposition
Surface chemistry
Catalysis
Cyclic voltammetry
Fourier Analysis
Surface treatment
Fourier transforms
Anodes
Ethylene
Durability
Infrared radiation
Lithium-ion batteries

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Shi, Feifei ; Ross, Philip N. ; Zhao, Hui ; Liu, Gao ; Somorjai, Gabor A. ; Komvopoulos, Kyriakos. / A catalytic path for electrolyte reduction in lithium-ion cells revealed by in situ attenuated total reflection-fourier transform infrared spectroscopy. In: Journal of the American Chemical Society. 2015 ; Vol. 137, No. 9. pp. 3181-3184.
@article{be3464c2cfd1492db2d01b1e695cfc56,
title = "A catalytic path for electrolyte reduction in lithium-ion cells revealed by in situ attenuated total reflection-fourier transform infrared spectroscopy",
abstract = "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.",
author = "Feifei Shi and Ross, {Philip N.} and Hui Zhao and Gao Liu and Somorjai, {Gabor A.} and Kyriakos Komvopoulos",
year = "2015",
month = "2",
doi = "10.1021/ja5128456",
language = "English (US)",
volume = "137",
pages = "3181--3184",
journal = "Journal of the American Chemical Society",
issn = "0002-7863",
publisher = "American Chemical Society",
number = "9",

}

A catalytic path for electrolyte reduction in lithium-ion cells revealed by in situ attenuated total reflection-fourier transform infrared spectroscopy. / Shi, Feifei; Ross, Philip N.; Zhao, Hui; Liu, Gao; Somorjai, Gabor A.; Komvopoulos, Kyriakos.

In: Journal of the American Chemical Society, Vol. 137, No. 9, 02.2015, p. 3181-3184.

Research output: Contribution to journalArticle

TY - JOUR

T1 - A catalytic path for electrolyte reduction in lithium-ion cells revealed by in situ attenuated total reflection-fourier transform infrared spectroscopy

AU - Shi, Feifei

AU - Ross, Philip N.

AU - Zhao, Hui

AU - Liu, Gao

AU - Somorjai, Gabor A.

AU - Komvopoulos, Kyriakos

PY - 2015/2

Y1 - 2015/2

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=84924674718&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84924674718&partnerID=8YFLogxK

U2 - 10.1021/ja5128456

DO - 10.1021/ja5128456

M3 - Article

AN - SCOPUS:84924674718

VL - 137

SP - 3181

EP - 3184

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 9

ER -