High‐Yield Preparation, Versatile Structural Modification, and Properties of Layered Cobalt Hydroxide Nanocones

A low‐cost oil bath synthetic route is presented to produce uniform and highly crystalline layered cobalt hydroxide nanocones (NCs) intercalated with dodecyl sulfate anions (C₁₂H₂₅OSO₃⁻, DS⁻). A new exfoliating procedure, by gradually unravelling/unzipping these NCs through heat treatment in formamide‐water binary solution, is developed to prepare unilamellar nanosheets. Moreover, the NCs can be readily modified with various inorganic or organic anions via a conventional anion‐exchange process at ambient temperature. The exchanged product, for example, NO₃⁻–intercalated NCs, can be more easily and rapidly transformed into cobalt oxides (e.g., Co₃O₄ and CoO) than the original DS⁻–intercalated form while retaining a conical feature. Both the cobalt hydroxide NCs and exfoliated nanosheets are electrochemically redoxable, exhibiting a Faradaic pseudocapacitive behavior. The magnetic measurements further reveal both antiferromagnetic behaviors for transformed Co₃O₄ and CoO NCs. Their Néel temperature values are lower than those of bulk oxides due to finite size and geometric confinement effect. The peculiar conical feature of NCs with a hollow interior and tunable layer spacing, as well as exfoliated unilamellar nanosheets with all surface area exposed, may show promise for potential applications in electrochemical energy storage and magnetic devices.