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For the first time, the detailed structure of χ-Al 2 O 3  and η-Al 2 O 3  surface has been established by implementing the NMR crystallography approach. The surface of η-Al 2 O 3  has been demonstrated to be formed primarily by the (111) facets, while the χ-Al 2 O 3  surface is a combination of (111) and (110) facets. This observation supports the block model of aluminum oxides previously proposed by Tsybulya and Kryukova [S. V. Tsybulya, G. N. Kryukova, Phys. Rev. B 77 (2008) 024112.]. The additional terminal OH groups, observed experimentally and not contributing to (111) and (110) theoretical calculations, are considered to be bonded to the tetrahedral aluminum sites. Their origin is related to the junctions of crystallographic faces of spinel building blocks, being a part of discussed model. Higher content of these terminal OH groups in χ-Al 2 O 3  is a result of more junctions in the case of its more mosaic structure compared to η-Al 2 O 3 .

Surface Hydroxyl OH Defects of η-Al 2 O 3 and χ-Al 2 O 3 by Solid State NMR, XRD, and DFT Calculations