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Title: Facile In Situ Syntheses of Cathode Protective Electrolyte Additives for High Energy Density Li-Ion Cells.

Abstract

Increasing the energy densities of Li-ion batteries necessitates operation of layered lithiated oxide cathodes at potentials exceeding 4 V vs Li/Li+. When continually exposed to such high potentials, these materials gradually deteriorate unless protected by sacrificial agents called electrolyte additives. During the formation cycles, these electrolyte additives decompose on the electrodes forming thin protective layers of insoluble products impeding further deleterious reactions. Some of these electrolyte additives spontaneously react when introduced into the electrolyte to yield specific surface-modifying products that alone protect the cathode; in other words, the nominal additive is the precursor and the secondary product is the protective agent. Guided by this insight, we used molecular engineering to obtain such surface-active secondary products in situ with 100% yield. Two of these electrolyte additives proved exceptional in that they delay both the impedance rise and capacity fade in the Li-ion cells. We demonstrate this protective action and scrutinize the activation of these additives in the electrolyte. By "taming" spontaneous reactions and regaining full control over the chemical structure, new avenues open to targeted synthesis of electrolyte additives extending the operation of high voltage Li-ion batteries.

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE) - Office of Vehicle Technologies (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1531165
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 7
Country of Publication:
United States
Language:
English

Citation Formats

Shkrob, Ilya A., Han, Binghong, Sahore, Ritu, Tornheim, Adam P., Zhang, Lu, Abraham, Daniel P, Dogan, Fulya, Zhang, Zhengcheng, and Liao, Chen. Facile In Situ Syntheses of Cathode Protective Electrolyte Additives for High Energy Density Li-Ion Cells.. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.8b05261.
Shkrob, Ilya A., Han, Binghong, Sahore, Ritu, Tornheim, Adam P., Zhang, Lu, Abraham, Daniel P, Dogan, Fulya, Zhang, Zhengcheng, & Liao, Chen. Facile In Situ Syntheses of Cathode Protective Electrolyte Additives for High Energy Density Li-Ion Cells.. United States. doi:10.1021/acs.chemmater.8b05261.
Shkrob, Ilya A., Han, Binghong, Sahore, Ritu, Tornheim, Adam P., Zhang, Lu, Abraham, Daniel P, Dogan, Fulya, Zhang, Zhengcheng, and Liao, Chen. Tue . "Facile In Situ Syntheses of Cathode Protective Electrolyte Additives for High Energy Density Li-Ion Cells.". United States. doi:10.1021/acs.chemmater.8b05261.
@article{osti_1531165,
title = {Facile In Situ Syntheses of Cathode Protective Electrolyte Additives for High Energy Density Li-Ion Cells.},
author = {Shkrob, Ilya A. and Han, Binghong and Sahore, Ritu and Tornheim, Adam P. and Zhang, Lu and Abraham, Daniel P and Dogan, Fulya and Zhang, Zhengcheng and Liao, Chen},
abstractNote = {Increasing the energy densities of Li-ion batteries necessitates operation of layered lithiated oxide cathodes at potentials exceeding 4 V vs Li/Li+. When continually exposed to such high potentials, these materials gradually deteriorate unless protected by sacrificial agents called electrolyte additives. During the formation cycles, these electrolyte additives decompose on the electrodes forming thin protective layers of insoluble products impeding further deleterious reactions. Some of these electrolyte additives spontaneously react when introduced into the electrolyte to yield specific surface-modifying products that alone protect the cathode; in other words, the nominal additive is the precursor and the secondary product is the protective agent. Guided by this insight, we used molecular engineering to obtain such surface-active secondary products in situ with 100% yield. Two of these electrolyte additives proved exceptional in that they delay both the impedance rise and capacity fade in the Li-ion cells. We demonstrate this protective action and scrutinize the activation of these additives in the electrolyte. By "taming" spontaneous reactions and regaining full control over the chemical structure, new avenues open to targeted synthesis of electrolyte additives extending the operation of high voltage Li-ion batteries.},
doi = {10.1021/acs.chemmater.8b05261},
journal = {Chemistry of Materials},
number = 7,
volume = 31,
place = {United States},
year = {2019},
month = {4}
}