1：Experimental Design and Method Selection:

Density functional theory (DFT) calculations were performed using the Vienna ab initio simulation package (VASP) with projector augmented wave pseudopotentials and Perdew-Burke-Ernzerhof generalized gradient approximation. The climbing nudged elastic band (NEB) method was used for activation energy calculations, and the HSE06 functional was employed for electronic structure evaluation.

2：Sample Selection and Data Sources:

Layered ReS2 crystals were chosen as the model system due to their distorted diamond-chain structure and charge decoupling properties. Structures with intercalated alkali-metal atoms (Li, Na, K) were constructed and optimized.

3：List of Experimental Equipment and Materials:

Computational software VASP was used; no physical equipment or materials are mentioned.

4：Experimental Procedures and Operational Workflow:

Structures were optimized with a vacuum space of 20 ?, energy cutoff of 450 eV, and Monkhorst-Pack k-point meshes of 9×9×1. Formation energies, band structures, density of states, phonon dispersions, and Gibbs free energies were calculated under various strains and intercalation conditions.

5：Formation energies, band structures, density of states, phonon dispersions, and Gibbs free energies were calculated under various strains and intercalation conditions. Data Analysis Methods:

5. Data Analysis Methods: Data were analyzed using DFT-based methods, including calculation of formation energies, band gaps, charge density differences, and reaction free energies (ΔG = ΔE + ΔZPE - TΔS).