Using Molecular Dynamics to quantify the electrical double layer and examine the potential for its direct observation in the in-situ TEM
Abstract
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:
-
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Fundamental Computational Sciences Directorate
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1184294
- Report Number(s):
- PNNL-SA-106479
KC0208010
- Grant/Contract Number:
- AC05-76RL01830
- Resource 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
- 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
Citation Formats
Welch, David A., Mehdi, Beata L., Hatchell, Hanna J., Faller, Roland, Evans, James E., and Browning, Nigel D. Using Molecular Dynamics to quantify the electrical double layer and examine the potential for its direct observation in the in-situ TEM. United States: N. p., 2015.
Web. doi:10.1186/s40679-014-0002-2.
Welch, David A., Mehdi, Beata L., Hatchell, Hanna J., Faller, Roland, Evans, James E., & Browning, Nigel D. Using Molecular Dynamics to quantify the electrical double layer and examine the potential for its direct observation in the in-situ TEM. United States. https://doi.org/10.1186/s40679-014-0002-2
Welch, David A., Mehdi, Beata L., Hatchell, Hanna J., Faller, Roland, Evans, James E., and Browning, Nigel D. Wed .
"Using Molecular Dynamics to quantify the electrical double layer and examine the potential for its direct observation in the in-situ TEM". United States. https://doi.org/10.1186/s40679-014-0002-2. https://www.osti.gov/servlets/purl/1184294.
@article{osti_1184294,
title = {Using Molecular Dynamics to quantify the electrical double layer and examine the potential for its direct observation in the in-situ TEM},
author = {Welch, David A. and Mehdi, Beata L. and Hatchell, Hanna J. and Faller, Roland and Evans, James E. and Browning, Nigel D.},
abstractNote = {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.},
doi = {10.1186/s40679-014-0002-2},
journal = {Advanced Structural and Chemical Imaging, 1(1):Article No. 1},
number = ,
volume = ,
place = {United States},
year = {Wed Mar 25 00:00:00 EDT 2015},
month = {Wed Mar 25 00:00:00 EDT 2015}
}
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