Oxide/water interfaces are ubiquitous, with alumina/water drawing particular interest due to its environmental and industrial applications. Understanding the interfacial structure at the molecular level is crucial for many physical and chemical processes occurring there. However, the exact structure of interfacial H-bonded network at different pH values remains unclear. Here, sum-frequency vibrational spectroscopy in the OH stretch region was employed to study α-Al2O3 (0001)/water interface at different pH values, while suppressing the contribution of the diffusion layer by adding salts. The experimental results revealed although the variation of pH can charge the surface, it has little impact on the structure of the bonded interfacial layer (BIL). The interaction between alumina and water is mainly governed by weak hydrogen bonds. Furthermore, the templating effect of α-Al2O3 (0001) on the interfacial H-bonded network was observed, with the O–H stretch mode of ∼3430 cm−1 exhibiting anisotropy consistent with the (0001) surface symmetry. These findings indicate that the BIL structure on Al2O3 (0001) is predominantly influenced by the surface atom configuration, and the effect of charge changes induced by pH on the BIL structure is negligible.
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