Abstract
Transition metal trichalcogenides (TMTCs) of Group IVB (e.g., ZrS(3)) are promising lithium-ion battery (LIB) anodes owing to their tunable band gaps, anisotropic conductivity, and high specific capacities. Here, microsized ZrS(3) with a quasi-1D chain-based structure and van der Waals stacked layers were synthesized via a simple solid-state reaction. Subsequently, the ZrS(3) anode was evaluated across distinct voltage windows, the storage mechanism switched from intercalation (≥1.0 V) to conversion (down to 0.001 V). The ZrS(3) electrode delivers a high capacity of 844 mAh g(-1) at 50 mA g(-1) after 40 cycles, with excellent rate capability (281 mAh g(-1) at 3000 mA g(-1)) and outstanding cycling stability, maintaining 408 mAh g(-1) over 2300 cycles at 3000 mA g(-1). Ex situ XRD/SEM-EDX/XPS track phase and surface evolution, while EIS resolves interfacial charge-transfer/ion-transport kinetics. DFT reveals low-barrier Li(+) diffusion along interchain pathways in bulk (≈0.12 eV) and monolayer ZrS(3). A directional increase in the calculated Young's modulus under small strain suggests robust mechanics upon cycling. These experimental-theoretical insights establish ZrS(3) as a low-potential, high-rate anode for lithium-ion batteries and clarify the intercalation-conversion crossover in Group IVB TMTCs.