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Title: Using Molecular Dynamics to quantify the electrical double layer and examine the potential for its direct observation in the in-situ TEM

Understanding the fundamental processes taking place at the electrode-electrolyte interface in batteries will play a key role in the development of next generation energy storage technologies. One of the most fundamental aspects of the electrode-electrolyte interface is the electrical double layer (EDL). Given the recent development of high spatial resolution in-situ electrochemical cells for scanning transmission electron microscopy (STEM), there now exists the possibility that we can directly observe the formation and dynamics of the EDL. In this paper we predict electrolyte structure within the EDL using classical models and atomistic Molecular Dynamics (MD) simulations. The MD simulations show that the classical models fail to accurately reproduce concentration profiles that exist within the electrolyte. It is thus suggested that MD must be used in order to accurately predict STEM images of the electrode-electrolyte interface. Using MD and image simulations together for a high contrast electrolyte (the high atomic number CsCl electrolyte), it is determined that, for a smooth interface, concentration profiles within the EDL should be visible experimentally. When normal experimental parameters such as rough interfaces and low-Z electrolytes (like those used in Li-ion batteries) are considered, observation of the EDL appears to be more difficult.
Authors:
;  [1] ; ; ; ;
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Fundamental Computational Sciences Directorate
Publication Date:
OSTI Identifier:
1184294
Report Number(s):
PNNL-SA-106479
KC0208010
Grant/Contract Number:
AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
Advanced Structural and Chemical Imaging, 1(1):Article No. 1
Additional Journal Information:
Journal Name: Advanced Structural and Chemical Imaging, 1(1):Article No. 1
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 25 ENERGY STORAGE Image simulation; atomistic model; Molecular Dynamics; in-situ microscopy; electrochemistry; electrical double layer; N12994