TY - JOUR
T1 - Unraveling the New Role of an Ethylene Carbonate Solvation Shell in Rechargeable Metal Ion Batteries
AU - Li, Qian
AU - Cao, Zhen
AU - Wahyudi, Wandi
AU - Liu, Gang
AU - Park, Geon-Tae
AU - Cavallo, Luigi
AU - Anthopoulos, Thomas D.
AU - Wang, Limin
AU - Sun, Yang-Kook
AU - Alshareef, Husam N.
AU - Ming, Jun
N1 - KAUST Repository Item: Exported on 2020-12-16
Acknowledgements: This work is supported by the National Natural Science Foundation of China (21978281, 21975250) and the National Key R&D Program of China (SQ2017YFE9128100). The authors also thank the Independent Research Project of the State Key Laboratory of Rare Earth Resources Utilization (110005R086), Changchun Institute of Applied Chemistry, Chinese Academy of Sciences. The research was also supported by King Abdullah University of Science and Technology (KAUST) and Hanyang University.
PY - 2020/12/7
Y1 - 2020/12/7
N2 - Electrolytes play a critical role in controlling metal-ion battery performance. However, the molecular behavior of electrolyte components and their effects on electrodes are not fully understood. Herein, we present a new insight on the role of the most commonly used ethylene carbonate (EC) cosolvent both with the bulk and at the electrolyte-electrode interface. We have discovered a new phenomenon that contributes to stabilizing the electrolyte, besides the well-known roles of dissociating metal salt and forming a solid electrolyte interphase (SEI). As a paradigm, we confirm that EC can form an Li+–EC pair in a priority compared to other kinds of solvents (e.g., ethyl methyl carbonate) and then alter the Li+–solvent interactions in the electrolyte. The Li+–EC pair can dominate the desolvation structure at the electrode interface, therefore suppressing Li+–solvent decomposition due to the higher stability of Li+–EC. Our viewpoint is confirmed in different electrolytes for lithium, sodium, and potassium ion batteries, where the SEI is shown to be limited for stabilizing the electrode in the case of the less stable Li+–solvent pair. Our discovery provides a general explanation for the effect of EC and provides new guidelines for designing more reliable electrolytes for metal (ion) batteries.
AB - Electrolytes play a critical role in controlling metal-ion battery performance. However, the molecular behavior of electrolyte components and their effects on electrodes are not fully understood. Herein, we present a new insight on the role of the most commonly used ethylene carbonate (EC) cosolvent both with the bulk and at the electrolyte-electrode interface. We have discovered a new phenomenon that contributes to stabilizing the electrolyte, besides the well-known roles of dissociating metal salt and forming a solid electrolyte interphase (SEI). As a paradigm, we confirm that EC can form an Li+–EC pair in a priority compared to other kinds of solvents (e.g., ethyl methyl carbonate) and then alter the Li+–solvent interactions in the electrolyte. The Li+–EC pair can dominate the desolvation structure at the electrode interface, therefore suppressing Li+–solvent decomposition due to the higher stability of Li+–EC. Our viewpoint is confirmed in different electrolytes for lithium, sodium, and potassium ion batteries, where the SEI is shown to be limited for stabilizing the electrode in the case of the less stable Li+–solvent pair. Our discovery provides a general explanation for the effect of EC and provides new guidelines for designing more reliable electrolytes for metal (ion) batteries.
UR - http://hdl.handle.net/10754/666391
UR - https://pubs.acs.org/doi/10.1021/acsenergylett.0c02140
U2 - 10.1021/acsenergylett.0c02140
DO - 10.1021/acsenergylett.0c02140
M3 - Article
SN - 2380-8195
SP - 69
EP - 78
JO - ACS Energy Letters
JF - ACS Energy Letters
ER -