The issues during Zn deposition in rechargeable Zn-based
batteries
greatly hinder cycling stability. In this work, a simple and inexpensive
approach to tailor the Zn electrodeposition is proposed by tuning
the viscosity of the liquid electrolyte (LE). First, the growth mechanisms
of Zn deposition under different electrolyte properties are investigated
by numerical simulation, from which the bottom deposition tends to
fuse with each other when there are more deposition sites, and the
mass-transfer coefficient is lower, thus achieving uniform deposition.
Besides, the whole process of Zn deposition in charging–discharging
cycling is in situ observed by an optical microscope. It is found
that the cause of the poor stability in the LE is due to the uneven
Zn deposition, resulting in weak bonding between the deposition and
the electrode surface, which is also the reason for the formation
of dead Zn. In contrast, when an appropriate amount of the polymer
is added to the LE to increase the viscosity, an appropriate overpotential
can be created, generating more deposition sites. In addition, the
viscosity reduces the mass-transfer coefficient, making the distance
from the ion to the deposition sites the main controlling factor.
The Zn ions are more inclined to move in the direction of electric
field lines, which results in a uniform and dense deposition layer.
Furthermore, the effectiveness of this method is demonstrated in a
Zn–LiFePO4 battery, from which the battery with
the modified electrolyte condition still works properly even in the
Zn utilization of 100% and shows a capacity retention rate (35%) of
nearly twice that in the original LE condition (18%) after 10 cycles.
This work provides a theoretical basis for Zn deposition and provides
ideas for the future development of high-performance Zn-based batteries.