Synthesis of Low-Symmetric α‑Cobalt(II) Hydroxide-Incorporated Cyanuric Acid Layers with High Néel Temperature and Large Coercivity: Structure and Magnetism

α-Cobalt­(II) (CoII) hydroxide (compound 1) incorporating cyanuric acid layers was synthesized via the solvothermal method. 1 exhibited two distinct characteristics, which were different from reported α-CoII hydroxides. (i) The presence of abundant consecutive hydrogen bonds between the adjacent hydroxide layers enhanced the driving force of crystallization along the direction of the c axis. Thus, 1 revealed high crystallinity without the disorder phenomenon. (ii) 1 showed low symmetry. The configuration of CoTd sites did not follow the regular triangular net. The low symmetry favored the magnetic anisotropy. Thus, 1 revealed ferrimagnetic behavior with a high Néel temperature (T N = 56.8 K) and coercivity (H c = 36 kOe at 2 K). The ferrimagnetic behavior of 1 was validated via the Hubbard U correction density functional theory.