Dataset of "Quasi-1D Chain-Based Zirconium Trisulfide as a Low-Potential High-Rate Anode: Structural and Reaction Mechanism Insights"

Materials from the Group IVB transition metal trichalcogenides (TMTCs) family, such as zirconium trisulfide (ZrS3), have attracted significant attention for lithium-ion battery (LIB) applications due to their tunable band gaps, anisotropic conductivity, and high specific capacities. While several theoretical and experimental studies have focused on the synthesis and physicochemical properties of ZrS3, investigations into their lithium-ion storage properties have been limited. Herein, Micro-sized ZrS3 with a quasi-one-dimensional (quasi-1D) layered structure prepared using a straightforward solid-state reaction, were synthesized and evaluated as anode materials for LIBs to understand their electrochemical reaction mechanisms and structural evolution. Galvanostatic charge/discharge and cyclic voltammetry tests at various discharge depths (1.0, 0.3, and 0.001 V) were performed to characterize the transition between intercalation and conversion reactions. After 40 cycles, the ZrS3 electrodes displayed a high discharge capacity of 844 mAh g⁻¹ at a current density of 40 mA g⁻¹. In addition, they exhibited excellent rate capability, delivering a capacity of 281 mAh g⁻¹ at a high current density of 3000 mA g⁻¹ by the 40th cycle, along with remarkable long-term cycling stability over 2300 cycles, maintaining a stable capacity of 408 mAh g⁻¹. Furthermore, structural changes and surface evolution in the ZrS3 electrodes, observed under various electrochemical states through ex-situ characterization (XRD, SEM, SEM-EDX, cross section SEM, XPS and EIS), provided detailed insights into the electrochemical reaction processes. DFT calculations further elucidated the Li-ion diffusion pathways and energy barriers in both bulk and monolayer ZrS3, revealing intrinsic structural advantages that facilitate superior electrochemical performance. Our foundational study, combining detailed experimental analysis with theoretical insights, provides critical guidance for exploring electrochemical capabilities and rationally designing advanced Group IVB TMTC-based anode materials for alkali-ion batteries.