CrB4 crystallizes in the orthorhombic Immm space group. The structure is three-dimensional. Cr6+ is bonded to twelve equivalent B+1.50- atoms to form a mixture of face and edge-sharing CrB12 cuboctahedra. There are four shorter (2.09 Å) and eight longer (2.21 Å) Cr–B bond lengths. B+1.50- is bonded in a 7-coordinate geometry to three equivalent Cr6+ and four equivalent B+1.50- atoms. There are a spread of B–B bond distances ranging from 1.73–1.85 Å.
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