Designing zincophilic and stable carbon nanostructures
is critical
for Zn-ion storage with superior capacitive activity and durability.
Here, we report solvent-guided Lewis acid–base self-assembly
to customize heterodiatomic carbon nanotubes, triggered by the reaction
between iron chloride and α,α′-dichloro-p-xylene. In this strategy, modulating the solvent–precursor
interaction through the optimization of solvent formula stimulates
differential thermodynamic solubilization, growth kinetics, and self-assembly
behaviors of Lewis polymeric chains, thereby accurately tailoring
carbon nanoarchitectures to evoke superior Zn-ion storage. Featured
with open hollow interiors and porous tubular topologies, the solvent-optimized
carbon nanotubes allow low ion-migration barriers to deeply access
the built-in zincophilic sites by high-kinetics physical Zn2+/CF3SO3
– adsorption and robust
chemical Zn2+ redox with pyridine/carbonyl motifs, which
maximizes the spatial capacitive charge storage density. Thus, as-designed
heterodiatomic carbon nanotube cathodes provide all-round improvement
in Zn-ion storage, including a high energy density (140 W h kg–1), a large current activity (100 A g–1), and an exceptional long-term cyclability (100,000 cycles at 50
A g–1). This study provides appealing insights into
the solvent-mediated Lewis pair self-assembly design of nanostructured
carbons toward advanced Zn-ion energy storage.