Synergistic Amorphization and Interfacial Metallization Activates a Mn(VO₃)₂ Cathode with a Tailored Atomic-Layer Semimetallic 1T'-MoS₂ Interphase for Advanced Aqueous Zinc-Ion Batteries.

Abstract

Crystal Mn(VO₃)₂ (<i>c</i>-MVO) cathodes for aqueous zinc-ion batteries (AZIBs) typically experience irreversible structural degradation and slow Zn²⁺ diffusion kinetics. Here, we propose a colloidal chemical synthesis strategy that concurrently achieves amorphization and interphase engineering, constructing <i>a</i>-MVO@MoS₂ core@shell heterostructures. The <i>in situ</i> grown atomic-layer semimetallic 1T'-MoS₂ shell facilitates <i>a</i>-MVO formation and constructs a conductive interphase for faster electron transport, while a <i>a</i>-MVO core provides abundant Zn²⁺ reaction sites and flexible diffusion paths. Density functional theory calculations confirm that the diffusion barrier of Zn²⁺ in <i>a</i>-MVO@MoS₂ (1.08 eV) is considerably lower than that in <i>c</i>-MVO (3.71 eV). Consequently, the tailored <i>a</i>-MVO@MoS₂ cathode delivers a specific capacity of 205.68 mAh g^-1 at 0.5 A g^-1 (40 times that of <i>c</i>-MVO) and exhibits excellent cycling stability with a capacity retention of 87.64% after 5000 cycles at 10 A g^-1. This work paves a crystal phase engineering approach for designing advanced electrode materials for AZIBs.