Polymorphs of the Gadolinite-Type Borates ZrB2 O5 and HfB2 O5 Under Extreme Pressure

Chemistry. 2021 Apr 1;27(19):6007-6014. doi: 10.1002/chem.202005244. Epub 2021 Mar 3.

Abstract

Based on the results from previous high-pressure experiments on the gadolinite-type mineral datolite, CaBSiO4 (OH), the behavior of the isostructural borates β-HfB2 O5 and β-ZrB2 O5 have been studied by synchrotron-based in situ high-pressure single-crystal X-ray diffraction experiments. On compression to 120 GPa, both borate layer-structures are preserved. Additionally, at ≈114 GPa, the formation of a second phase can be observed in both compounds. The new high-pressure modification γ-ZrB2 O5 features a rearrangement of the corner-sharing BO4 tetrahedra, while still maintaining the four- and eight-membered rings. The new phase γ-HfB2 O5 contains ten-membered rings including the rare structural motif of edge-sharing BO4 tetrahedra with exceptionally short B-O and B⋅⋅⋅B distances. For both structures, unusually high coordination numbers are found for the transition metal cations, with ninefold coordinated Hf4+ , and tenfold coordinated Zr4+ , respectively. These findings remarkably show the potential of cold compression as a low-energy pathway to discover metastable structures that exhibit new coordinations and structural motifs.

Keywords: borates; diamond anvil cell; gadolinite structure; high-pressure chemistry; synchrotron radiation.