All-Round Enhancement in Zn-Ion Storage Enabled by Solvent-Guided Lewis Acid–Base Self-Assembly of Heterodiatomic Carbon Nanotubes

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.