Data for "Self-assembled polyelectrolytes with ion-separation accelerating channels for highly stable Zn-ion batteries"

Aqueous zinc-ion batteries (AZIBs) are increasingly recognized as a sustainable alternative to lithium-ion batteries (LIBs) due to their abundance, safety, and lower environmental impact. However, the hydrogen evolution reaction (HER) and uncontrolled diffusion of Zn²⁺ and SO₄^2- ions lead to the dendrite formation and side reactions, which hinder their practical application by forming a non-conductive layer on the Zn anode. This layer impedes the ion transport and electron flow, reducing the Coulombic efficiency (CE) for the Zn nucleation. Here, to simultaneously regulate the diffusion of H⁺, Zn²⁺, and SO₄^2- in the electrolyte, an ion-separation accelerating channel was constructed to unify the Zn deposition by introducing an eco-friendly layer-by-layer self-assembly of a flocculant poly(allylamine hydrochloride) (PAH) and its tautomer poly(acrylic acid) (PAA). The dual-ion channels, created by strong electrostatic interactions between carboxylate anions (COO⁻) and ammonia cations (NH₃⁺), block SO₄^2- and promote the uniform Zn deposition along the (002) plane, exhibiting a CE of 99.8% after 1600 cycles in the Zn||Cu asymmetric cell. With the facile fabrication of the layer-by-layer self-assembled Zn anode, an Ah-level pouch cell (17.36 Ah) with a high mass loading (> 8 mg cm⁻²) demonstrated the practical viability for large-scale applications, retaining a capacity of 93.6% for at least 250 cycles at 1.7 C. This innovation not only enables faster and more uniform Zn deposition but also significantly enhances the cycling stability and mechanical durability in larger pouch cells, paving the way for the commercialization of AZIBs.