For the pristine COF-1 material (no solvent), we generated AIMD trajectories with two different setups using either k-point (KP) meshes or large supercells (SC). In the KP setup, our computational model is a COF-1 unit cell, i.e., a structure with 84 atoms shown in Figure , in combination with a 1 × 1 × 3 k-point grid. For the SC setup, we used a 1 × 1 × 2 COF-1 supercell, which contains 4 layers and 168 atoms (see Figure ), and performed all electronic-structure calculations at the Γ-point only. In order to investigate the solvent effects, we generated a third AIMD trajectory using a 1 × 1 × 3 COF-1 supercell with 1,4-dioxane molecules in the pores, see Figures and. The initial COF-1+solvent structure was generated with the PACKMOL package, setting a density of 1.033 g/mL for the solvent. The COF-1+solvent supercell contains seven 1,4-dioxane molecules in the pores, resulting in a system size of 350 atoms. The AIMD starting structures were cell-and geometry optimized at the PBE+TS level with FHI-aims.