Universality of Lithium Metal and Solid Electrolyte Interphase Descriptors of Coulombic Efficiency Governed by Lithium Connectivity
- 1Department of Mechanical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts, 02139
Abstract
Coulombic efficiency (CE) is a key metric governing the cyclability of lithium metal anodes, motivating efforts to identify physicochemical descriptors that correlate with CE. Diverse descriptors spanning electrolyte thermodynamics and interphase properties have been proposed, but their interrelationships and underlying physical origins remain unclear. Here we show that, when evaluated across a consistent electrolyte set, these descriptors exhibit a common hockey-stick relationship with CE that can be unified through the mesoscale connectivity of lithium deposits. A percolation-like transition from isolated deposits to interconnected networks sharply suppresses inactive Li0 formation during stripping, which underlies the common CE transition across descriptors. Tuning plating current density reproduces this transition within individual electrolytes, demonstrating that connectivity is not uniquely determined by electrolyte chemistry. These findings establish lithium connectivity as a common mechanistic basis for diverse CE correlations and provide a framework for interpreting these correlations across distinct capacity-loss regimes.
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BibTeX
@misc{kim2026universality,
title = {{Universality of Lithium Metal and Solid Electrolyte Interphase Descriptors of Coulombic Efficiency Governed by Lithium Connectivity}},
author = {Jihyeon Kim and Betar Gallant},
howpublished = {ChemRxiv},
year = {2026},
month = oct,
doi = {10.26434/chemrxiv.15010842/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15010842/v1},
note = {CC BY-NC-ND},
}
RIS
TY - UNPB
TI - Universality of Lithium Metal and Solid Electrolyte Interphase Descriptors of Coulombic Efficiency Governed by Lithium Connectivity
AU - Jihyeon Kim
AU - Betar Gallant
PY - 2026
DA - 2026/10/22
PB - ChemRxiv
DO - 10.26434/chemrxiv.15010842/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15010842/v1
AB - Coulombic efficiency (CE) is a key metric governing the cyclability of lithium metal anodes, motivating efforts to identify physicochemical descriptors that correlate with CE. Diverse descriptors spanning electrolyte thermodynamics and interphase properties have been proposed, but their interrelationships and underlying physical origins remain unclear. Here we show that, when evaluated across a consistent electrolyte set, these descriptors exhibit a common hockey-stick relationship with CE that can be unified through the mesoscale connectivity of lithium deposits. A percolation-like transition from isolated deposits to interconnected networks sharply suppresses inactive Li0 formation during stripping, which underlies the common CE transition across descriptors. Tuning plating current density reproduces this transition within individual electrolytes, demonstrating that connectivity is not uniquely determined by electrolyte chemistry. These findings establish lithium connectivity as a common mechanistic basis for diverse CE correlations and provide a framework for interpreting these correlations across distinct capacity-loss regimes.
ER -