In this work, the authors present the free-standing multifunctional electrodes created by combining the atomic layer deposition of palladium (Pd) and nickel oxide (NiO) nanostructures directly onto gas diffusion electrodes (GDE) as multifunctional electrocatalyst for the hydrogen evolution reaction (HER), ethanol oxidation reaction (EtOR), and glycerol oxidation reaction (GOR) in both half-cell and hydroxide anion exchange membrane (AEM) electrolyzer configuration. However, the novelty and overall quality of this manuscript currently do not meet the standards required for publication in Journal of Materials Chemistry A.

1. The ALD process parameters (such as the deposition temperature of Pd and NiO, and the pulse time of the precursor) need to be further justified for their rationality. For instance, the quantitative relationship between the number of ALD cycles of NiO (250 vs. 1000) and the film thickness and catalytic performance has not been fully explored.

2. The optimization basis for hydrogen concentration (5% H2/Ar) and temperature (500°C) during the heat treatment process has not been clarified. Supplementary comparative experiments (such as the influence of different reduction temperatures on alloy formation) are needed to support the parameter selection.

3. The current 12-hour electrolysis test only verifies the short-term stability. However, in practical applications, the electrode needs to withstand long-term cycling conditions. It is recommended to supplement with 100-hour or more constant current/constant voltage cycling tests. Combined with SEM/XRD analysis of the electrode morphology and composition changes, the ability of the catalyst to resist sintering and corrosion should be evaluated.

4. The author suggests that the synergistic effect between NiO and Pd stems from the adjustment of electronic structure, but lacks direct evidence (such as DFT calculations) to reveal the mechanism of d-band center shift or charge transfer. It is recommended to supplement theoretical calculations to clarify the regulatory role of NiO on the electronic states of Pd.

5. The precise role of the Ni(OH)2/NiOOH redox couple in the EtOR/GOR processes requires further elucidation through in situ Raman or infrared spectroscopic analysis.