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Title: Investigation on the Charging Process of Li2O2-Based Air Electrodes in Li-O2 Batteries with Organic Carbonate Electrolytes

Abstract

The charge processes of Li-O2 batteries were investigated by analyzing the gas evolution by in situ gas chromatography-mass spectroscopy (GC/MS) technique. The mixture of Li2O2/Fe3O4/Super P carbon/polyvinylidene fluoride (PVDF) was used as the starting air electrode material and 1M LiTFSI in carbonate-based solvents was used as electrolyte. It was found that Li2O2 is reactive to 1-methyl-2-pyrrolidinone and PVDF binder used in the electrode preparation. During the 1st charge (up to 4.6 V), O2 was the main component in the gases released. The amount of O2 measured by GC/MS was consistent with the amount of Li2O2 decomposed in the electrochemical process as measured by the charge capacity, indicative of the good chargeability of Li2O2. However, after the cell was discharged to 2.0 V in O2 atmosphere and re-charged to ~ 4.6 V in the second cycle, CO2 was dominant in the released gases. Further analysis of the discharged air electrode by X-ray diffraction and Fourier transform infrared spectroscopy indicated that lithium-containing carbonate species (lithium alkyl carbonate and/or Li2CO3) were the main reaction products. Therefore, compatible electrolyte and electrodes as well as the electrode preparation procedures need to be developed for long term operation of rechargeable Li-O2 or Li-air batteries.

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1006292
Report Number(s):
PNNL-SA-75700
Journal ID: ISSN 0378-7753; TRN: US201105%%926
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Power Sources, 196(8):3894-3899
Additional Journal Information:
Journal Volume: 196; Journal Issue: 8; Journal ID: ISSN 0378-7753
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; METAL-NONMETAL BATTERIES; LITHIUM; OXYGEN; BATTERY CHARGING; LITHIUM OXIDES; IRON OXIDES; CARBON; ORGANIC POLYMERS; GASES; CHEMICAL COMPOSITION; Li-O2 battery; GC/MS technique; in situ analysis; Charge process; Gas evolution

Citation Formats

Xu, Wu, Viswanathan, Vilayanur V, Wang, Deyu, Towne, Silas A, Xiao, Jie, Nie, Zimin, Hu, Dehong, and Zhang, Jiguang. Investigation on the Charging Process of Li2O2-Based Air Electrodes in Li-O2 Batteries with Organic Carbonate Electrolytes. United States: N. p., 2011. Web. doi:10.1016/j.jpowsour.2010.12.065.
Xu, Wu, Viswanathan, Vilayanur V, Wang, Deyu, Towne, Silas A, Xiao, Jie, Nie, Zimin, Hu, Dehong, & Zhang, Jiguang. Investigation on the Charging Process of Li2O2-Based Air Electrodes in Li-O2 Batteries with Organic Carbonate Electrolytes. United States. https://doi.org/10.1016/j.jpowsour.2010.12.065
Xu, Wu, Viswanathan, Vilayanur V, Wang, Deyu, Towne, Silas A, Xiao, Jie, Nie, Zimin, Hu, Dehong, and Zhang, Jiguang. Fri . "Investigation on the Charging Process of Li2O2-Based Air Electrodes in Li-O2 Batteries with Organic Carbonate Electrolytes". United States. https://doi.org/10.1016/j.jpowsour.2010.12.065.
@article{osti_1006292,
title = {Investigation on the Charging Process of Li2O2-Based Air Electrodes in Li-O2 Batteries with Organic Carbonate Electrolytes},
author = {Xu, Wu and Viswanathan, Vilayanur V and Wang, Deyu and Towne, Silas A and Xiao, Jie and Nie, Zimin and Hu, Dehong and Zhang, Jiguang},
abstractNote = {The charge processes of Li-O2 batteries were investigated by analyzing the gas evolution by in situ gas chromatography-mass spectroscopy (GC/MS) technique. The mixture of Li2O2/Fe3O4/Super P carbon/polyvinylidene fluoride (PVDF) was used as the starting air electrode material and 1M LiTFSI in carbonate-based solvents was used as electrolyte. It was found that Li2O2 is reactive to 1-methyl-2-pyrrolidinone and PVDF binder used in the electrode preparation. During the 1st charge (up to 4.6 V), O2 was the main component in the gases released. The amount of O2 measured by GC/MS was consistent with the amount of Li2O2 decomposed in the electrochemical process as measured by the charge capacity, indicative of the good chargeability of Li2O2. However, after the cell was discharged to 2.0 V in O2 atmosphere and re-charged to ~ 4.6 V in the second cycle, CO2 was dominant in the released gases. Further analysis of the discharged air electrode by X-ray diffraction and Fourier transform infrared spectroscopy indicated that lithium-containing carbonate species (lithium alkyl carbonate and/or Li2CO3) were the main reaction products. Therefore, compatible electrolyte and electrodes as well as the electrode preparation procedures need to be developed for long term operation of rechargeable Li-O2 or Li-air batteries.},
doi = {10.1016/j.jpowsour.2010.12.065},
url = {https://www.osti.gov/biblio/1006292}, journal = {Journal of Power Sources, 196(8):3894-3899},
issn = {0378-7753},
number = 8,
volume = 196,
place = {United States},
year = {2011},
month = {4}
}