4.8 Article

Engineering an electrostatic field layer for high-rate and dendrite-free Zn metal anodes

Journal

ENERGY & ENVIRONMENTAL SCIENCE
Volume 16, Issue 8, Pages 3612-3622

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d3ee01724a

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In this study, an electrostatic field layer (EFL) was established using an electrolyte additive of cobalt tetraaminophthalocyanine (Co(TAPC)) to address the instability issue of the Zn metal/electrolyte interface, parasitic reactions, and dendritic growth, resulting in low Coulombic efficiency (CE) and poor cycle life. The Co(TAPC) with a planar and large conjugated ring structure could preferentially absorb on the Zn metal anode to form a zincophilic EFL, which prevents direct contact of Zn and water, suppresses side reactions, promotes desolvation and Zn2+ diffusion kinetics, and balances the space electric field, thereby enabling high-rate and dendrite-free Zn deposition.
Commercialization of zinc (Zn) metal batteries is significantly hindered by the instability of the Zn metal/electrolyte interface(s), together with concurrent parasitic reactions and dendritic growth that leads to low Coulombic efficiency (CE) and poor cycle life. Here, we report an electrostatic field layer (EFL) established via an electrolyte additive of cobalt tetraaminophthalocyanine (Co(TAPC)) to obviate these drawbacks. We confirm using judiciously combined experimental characterization and theoretical computation that Co(TAPC) with a planar and large conjugated ring structure preferentially absorbs on the Zn metal anode to form a zincophilic EFL, which prevents direct contact of Zn and water, suppresses side reaction(s), promotes desolvation and Zn2+ diffusion kinetics and balances the space electric field, thus enabling high-rate and dendrite-free Zn deposition. The Zn metal anode exhibits an ultra-long cycle life of >8000 cycles at a current density of 50 mA cm(-2) and high CE under harsh test conditions of 5 mA h cm(-2) and 10 mA cm(-2). Moreover, the utility of the Co(TAPC) EFL is also demonstrated in Zn||MnO2 full cells, exhibiting outstanding cycling stability of 5000 cycles at a high current density of 2000 mA g(-1). Generally, the construction of a zincophilic EFL realizes uniform dendrite-free deposition in aqueous Zn metal batteries and opens an avenue for the design of stable metal anodes for high-performance metal batteries.

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