Bulletin of the American Physical Society
APS March Meeting 2023
Volume 68, Number 3
Las Vegas, Nevada (March 5-10)
Virtual (March 20-22); Time Zone: Pacific Time
Session AA07: V: Precision Many Body Physics
5:00 AM–6:48 AM,
Monday, March 20, 2023
Room: Virtual Room 7
Sponsoring
Unit:
DCOMP
Chair: Chenan Wei, University of Massachusetts Amherst
Abstract: AA07.00006 : Dimers and solvent layering determine electrochemically relevant species at electrolyte interfaces in Ca/BH4/THF
6:24 AM–6:36 AM
Presenter:
Ana Sanz Matias
(Lawrence Berkeley National Laboratory)
Author:
Ana Sanz Matias
(Lawrence Berkeley National Laboratory)
The increasing demand of large-scale energy storage with improved performance, safety and sustainability for renewable variable energy sources and automotive applications drives the search for post-Li-ion batteries based on multivalent cation chemistries (e.g., Mg, Zn and Ca). However, strong solvation shells limit their electrochemical activity, resulting in large overpotentials.
We study Ca(BH4)2 in THF as a promising candidate, spurred on by recent studies of bulk electrolyte and electrode interface. Here we use metadynamics to explore the three-dimensional free energy landscape of a Ca/BH4/THF electrolyte at a neutral and negatively charged inert interface. Specifically, we show that dimers, dominant at bulk, provide the most likely route to ionic species through disproportionation. A combined approach that leverages focused Umbrella Sampling for specific local minima and unsupervised data mining of the trajectories reveals molecular details of populations of distinct coordination environments; e.g., the rich isomerism of dimer structures. We find that the interfacial ionic species seem to respect the underlying solvent structure, resulting in a discretization of permitted interfacial dipole orientations and a modified disproportionation pathway. Furthermore, present the key finding that thermodynamic shifts and favors the monocation at the negative electrode but with a reversal of polarity.
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