Aqueous alkaline zinc batteries are of scientific and
technological
interest because of the potential they offer for cost-effective and
safe storage of electrical energy. Poor electrochemical reversibility
and shape change of the Zn anode, propensity of Zn to become passivated
by surface oxides and hydroxide films upon prolonged exposure to the
electrolyte, and electroreduction of water are well-studied but remain
unsolved challenges. Here, we create and study electrochemical and
transport properties of precise, spatially tunable zwitterionic polymer
interphases grown directly on Zn using an initiated-chemical vapor
deposition polymerization methodology. In aqueous alkaline media,
spatial gradients in compositionfrom the polymer–electrolyte
interface to the solid–polymer interfacepromote highly
reversible redox reactions at high current density (20 mA cm–2) and high areal capacity (10 mAh cm–2). Via molecular dynamics and experimental analyses, we conclude
that the interphases function by regulating the distribution and activity
of interfacial water molecules, which simultaneously enables fast
ion transport and suppression of surface passivation and the hydrogen
evolution reaction. To illustrate the practical relevance of our findings,
we study aqueous Zn||NiOOH and Zn||air batteries and observe that
zwitterionic polymer interphases produce extended life at high currents
and high areal capacity.
In this work, we employ large-scale coarse-grained molecular dynamics (CGMD) simulations to study the three-dimensional line edge roughness associated with line and space patterns of chemo-epitaxially directed symmetric block copolymers.
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