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Title: The Role of Cesium Cation in Controlling Interphasial Chemistry on Graphite Anode in Propylene Carbonate-Rich Electrolytes

Abstract

Propylene carbonate (PC) is seldom used in lithium-ion batteries (LIBs) due to its sustained co-intercalation into graphene structure and the eventual graphite exfoliation, despite potential advantages it brings, such as wider liquid range and lower cost. Here we discover that cesium cation (Cs+), originally used to suppress dendrite growth of Li metal anode, directs the formation of solid electrolyte interphase (SEI) on graphitic anode in PC-rich electrolytes through preferential solvation. Effective suppression of PC-decomposition and graphite-exfoliation was achieved when the ratio of ethylene carbonate (EC)/PC in electrolytes was so adjusted that the reductive decomposition of Cs+-(EC)m (1≤m≤2) complex precedes that of Li+-(PC)n (3≤n≤5). The interphase directed by Cs+ is stable, ultrathin and compact, leading to significant improvements in LIB performances. In a broader context, the accurate tailoring of SEI chemical composition by introducing a new solvation center represents a fundamental breakthrough in manipulating interfacial reactions processes that once were elusive.

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1222897
Report Number(s):
PNNL-SA-110487
48379; VT1201000
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
ACS Applied Materials & Interfaces, 7(37):20687-20695
Additional Journal Information:
Journal Name: ACS Applied Materials & Interfaces, 7(37):20687-20695
Country of Publication:
United States
Language:
English
Subject:
cesium cation; grapite anode; interfacial reactions; Environmental Molecular Sciences Laboratory

Citation Formats

Xiang, Hongfa, Mei, Donghai, Yan, Pengfei, Bhattacharya, Priyanka, Burton, Sarah D., Cresce, Arthur V., Cao, Ruiguo, Engelhard, Mark H., Bowden, Mark E., Zhu, Zihua, Polzin, Bryant, Wang, Chong M., Xu, Kang, Zhang, Jiguang, and Xu, Wu. The Role of Cesium Cation in Controlling Interphasial Chemistry on Graphite Anode in Propylene Carbonate-Rich Electrolytes. United States: N. p., 2015. Web. doi:10.1021/acsami.5b05552.
Xiang, Hongfa, Mei, Donghai, Yan, Pengfei, Bhattacharya, Priyanka, Burton, Sarah D., Cresce, Arthur V., Cao, Ruiguo, Engelhard, Mark H., Bowden, Mark E., Zhu, Zihua, Polzin, Bryant, Wang, Chong M., Xu, Kang, Zhang, Jiguang, & Xu, Wu. The Role of Cesium Cation in Controlling Interphasial Chemistry on Graphite Anode in Propylene Carbonate-Rich Electrolytes. United States. https://doi.org/10.1021/acsami.5b05552
Xiang, Hongfa, Mei, Donghai, Yan, Pengfei, Bhattacharya, Priyanka, Burton, Sarah D., Cresce, Arthur V., Cao, Ruiguo, Engelhard, Mark H., Bowden, Mark E., Zhu, Zihua, Polzin, Bryant, Wang, Chong M., Xu, Kang, Zhang, Jiguang, and Xu, Wu. Thu . "The Role of Cesium Cation in Controlling Interphasial Chemistry on Graphite Anode in Propylene Carbonate-Rich Electrolytes". United States. https://doi.org/10.1021/acsami.5b05552.
@article{osti_1222897,
title = {The Role of Cesium Cation in Controlling Interphasial Chemistry on Graphite Anode in Propylene Carbonate-Rich Electrolytes},
author = {Xiang, Hongfa and Mei, Donghai and Yan, Pengfei and Bhattacharya, Priyanka and Burton, Sarah D. and Cresce, Arthur V. and Cao, Ruiguo and Engelhard, Mark H. and Bowden, Mark E. and Zhu, Zihua and Polzin, Bryant and Wang, Chong M. and Xu, Kang and Zhang, Jiguang and Xu, Wu},
abstractNote = {Propylene carbonate (PC) is seldom used in lithium-ion batteries (LIBs) due to its sustained co-intercalation into graphene structure and the eventual graphite exfoliation, despite potential advantages it brings, such as wider liquid range and lower cost. Here we discover that cesium cation (Cs+), originally used to suppress dendrite growth of Li metal anode, directs the formation of solid electrolyte interphase (SEI) on graphitic anode in PC-rich electrolytes through preferential solvation. Effective suppression of PC-decomposition and graphite-exfoliation was achieved when the ratio of ethylene carbonate (EC)/PC in electrolytes was so adjusted that the reductive decomposition of Cs+-(EC)m (1≤m≤2) complex precedes that of Li+-(PC)n (3≤n≤5). The interphase directed by Cs+ is stable, ultrathin and compact, leading to significant improvements in LIB performances. In a broader context, the accurate tailoring of SEI chemical composition by introducing a new solvation center represents a fundamental breakthrough in manipulating interfacial reactions processes that once were elusive.},
doi = {10.1021/acsami.5b05552},
url = {https://www.osti.gov/biblio/1222897}, journal = {ACS Applied Materials & Interfaces, 7(37):20687-20695},
number = ,
volume = ,
place = {United States},
year = {2015},
month = {9}
}