This manuscript reported investigates the early-stage nucleation of lithium on different surface chemistries of the lithium metal anode using density functional theory. After careful evaluation of the manuscript, I recommend major revisions for the manuscript prior to publication in Materials Advances.
Major Comments:
1) The manuscript relies entirely on static 0 K DFT calculations, and the absence of finite-temperature, solvent/electrolyte, and electrochemical potential effects limits the applicability of the conclusions to realistic battery operating conditions.
2) The claim that fluorine defects promote uniform lithium deposition is overstated and should be supported by additional dynamic simulations (e.g., AIMD or kinetic Monte Carlo) or toned down accordingly.
3) The study considers only isolated O, N, and F defects, whereas realistic SEI contains complex multi-component interfaces (LiF, Li₂O, Li₂CO₃, Li₃N, organic species), which should be discussed as a limitation.
4) The manuscript lacks quantitative validation against available experimental nucleation overpotentials, cryo-TEM observations, or reported facet-dependent lithium deposition behavior to strengthen the computational findings.
5) Only low-index pristine facets are investigated; the omission of grain boundaries, surface roughness, high-index facets, and reconstructed surfaces limits the generality of the proposed nucleation mechanism.
6) The methodology requires additional justification regarding the selected exchange-correlation functional, slab thickness, vacuum spacing, and convergence tests to ensure the reliability of the calculated adsorption energies.
7) Although diffusion barriers are briefly discussed, the relationship between adsorption energetics, diffusion kinetics, and dendrite evolution remains qualitative and requires deeper mechanistic analysis.
8) The discussion should better distinguish between thermodynamic preference and kinetic accessibility, as favorable adsorption energies alone cannot fully predict dendrite nucleation behavior under practical electrochemical conditions.
9) The conclusions should be moderated because the current computational evidence does not fully substantiate the broad claims regarding defect engineering strategies for suppressing dendrite formation in practical lithium-metal batteries.

Accept.