Interplay Between Two Adjacent Electrical Double Layers at Metal | Solid Electrolyte | Liquid Electrolyte Interfaces

The Journal of Physical Chemistry C, vol. 128, pp. 14654–14662

Abstract

Electrical double layer (EDL) in modern batteries is radically different from that of the mercury electrode for which the conventional EDL models were initially developed. Particularly, the formation of a solid electrolyte interphase (SEI) divides the electrode–solution interface into two adjacent interfaces, while the interplay between these two EDLs is largely unclear. Herein, considering a metal | solid electrolyte | liquid electrolyte (M|SE|LE) system, we developed continuum models to understand the correlation between the charging states of the two adjacent EDLs. In addition to numerical results, analytical solutions of the differential double layer capacitances for two limiting cases, where the mobile charge countering the metal surface charge exists in either the SE or the LE, are obtained. The critical electrode potential marking the transition between the two limiting cases is analyzed. This work contributes to the understanding of nontraditional electrochemical interfaces in modern batteries.

Authors 6

1. Yupeng Qin

   Dalian Institute of Chemical Physics · Chinese Academy of Sciences · University of Chinese Academy of Sciences

   Affiliation as printed

   Laboratory of Advanced Spectro-electrochemistry and Li-ion Batteries, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

   University of the Chinese Academy of Sciences, Beijing 100049, China

2. Jun Zh. Huang corresponding Aachen Theory of Electrocatalytic Interfaces Faculty of Georesources and Materials Engineering

   Forschungszentrum Jülich · RWTH Aachen University

   Affiliation as printed

   IEK-13: Theory and Computation of Energy Materials, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich 52425, Germany

   Theory of Electrocatalytic Interfaces, Faculty of Georesources and Materials Engineering, RWTH Aachen University, Aachen 52062, Germany

3. Jie Zhang

   Dalian Institute of Chemical Physics · Chinese Academy of Sciences

   Affiliation as printed

   Laboratory of Advanced Spectro-electrochemistry and Li-ion Batteries, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

4. Zhiwei Zhao

   Dalian Institute of Chemical Physics · Chinese Academy of Sciences

   Affiliation as printed

   Laboratory of Advanced Spectro-electrochemistry and Li-ion Batteries, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

5. Limin Guo

   Dalian University

   Affiliation as printed

   College of Environment and Chemical Engineering, Dalian University, Dalian 116622, China

6. Zhangquan Peng corresponding

   Dalian Institute of Chemical Physics · Chinese Academy of Sciences

   Affiliation as printed

   Laboratory of Advanced Spectro-electrochemistry and Li-ion Batteries, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China