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Layered transition metal hydroxides (LTMHs) with transition metal centerssandwiched between layers of coordinating hydroxide anions have attractedconsiderable interest for their potential in developing clean energy sourcesand storage technologies. However, two dimensional (2D) LTMHs remain largelyunstudied in terms of their physical properties and the applications inelectronic devices. Here, directed by the relationship of the spin state of 3dtransition metal (TM) ions such as Ni, Co, Cu, and the corresponding geometryof the crystal field, we discover that Ni2+ with perfect Oh symmetry is idealfor intraplanar growth, leading to the achievement of >20 {\mu}m{\alpha}-Ni(OH)2 2D crystals with high yield, which are the largest 2D domainsreported so far. We also report the successful synthesis of 2D Co(OH)2 crystals(>40 {\mu}m) with less yield due to the slight geometry distortion resultedfrom uneven number of electrons. Moreover, the detailed structuralcharacterization of synthesized {\alpha}-Ni(OH)2 are performed; the opticalband gap energy is extrapolated as 2.54 eV from optical absorption measurementsand is measured as 2.50 eV from reflected electrons energy loss spectroscopy(REELS), suggesting the potential as insulating 2D dielectric material forelectronic devices. Furthermore, key parameters of the hydrothermal reactionincluding soaking temperature, starting pH and cooling rate, are systematicallytuned to understand their effects on morphological and crystallographicperspectives, allowing the establishment of a 2D growth mechanism. This workdemonstrates a scalable pathway to synthesize large 2D LTMHs from simplemethods, paving the way for the study of fundamental physical properties anddevice applications of 2D LTMHs.

Spin-state Directed Synthesis of >20 micrometers 2D Layered Transition Metal Hydroxides via Edge-on Condensation