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Download fileIn Situ Probing of Mass Exchange at the Solid Electrolyte Interphase in Aqueous and Nonaqueous Zn Electrolytes with EQCM‑D
journal contribution
posted on 2021-02-17, 19:36 authored by Saida Cora, Suzalmurni Ahmad, Niya SaMultivalent chemistry provides intriguing
benefits of developing
beyond lithium ion energy storage technologies and has drawn extensive
research interests. Among the multivalent candidates, metallic zinc
anodes offer an attractive high volumetric capacity at a low cost
for designing the secondary ion batteries. However, the interfacial
mass exchange at the Zn electrolyte/anode boundary is complicated.
The least understood solid electrolyte interphase (SEI) occurs simultaneously
with the reversible metal deposition, and its dynamic progression
is unclear and difficult to capture. One major challenge to investigate
such a dynamic interface is the lack of in situ analytical
methods that offer direct mass transport information to reproduce
the realistic battery operating conditions in an air-sensitive, nonaqueous
electrolyte environment with a high iR drop. Work
reported here reveals an in-depth analysis of the complex and dynamic
SEI at the Zn electrolyte/electrode interface utilizing a multiharmonic
quartz crystal microbalance with a dissipation method combined with
the spectroscopic analysis. Key differences are observed for the SEI
formation in the nonaqueous Zn(TFSI)2 electrolyte in contrast
to the aqueous ZnCl2 electrolyte for reversible Zn deposition.
A large disproportional loss of coulombs relative to the gravimetric
mass change is prominently observed at the initial electrochemical
cycles in the nonaqueous Zn electrolyte, and results suggest an in situ formation of an ionically permeable SEI layer that
is compositionally featured with a rich content of organic S and N
components. Further overtone-dependent dissipation analysis implies
the changes in viscoelasticity at the electrode interface during the
early SEI formation in the nonaqueous Zn(TFSI)2 electrolyte.
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Keywords
gravimetric mass changeZnCl 2 electrolyteSolid Electrolyte Interphasezinc anodes offernonaqueous Zn electrolytenonaqueous electrolyte environmentinterfacelithium ion energy storage technologiesEQCMmass transport informationmultiharmonic quartz crystal microb...Nonaqueous Zn ElectrolytesSEI formationovertone-dependent dissipation analysis