Controlling the Selective Formation of Calcium Sulfate Polymorphs at Room Temperature

Abstract Calcium sulfate is a naturally abundant and technologically important mineral with a broad scope of applications. However, controlling CaSO 4 polymorphism and, with it, its final material properties still represents a major challenge, and to date there is no universal method for the selective production of the different hydrated and anhydrous forms under mild conditions. Herein we report the first successful synthesis of pure anhydrite from solution at room temperature. We precipitated calcium sulfate in alcoholic media at low water contents. Moreover, by adjusting the amount of water in the syntheses, we can switch between the distinct polymorphs and fine‐tune the outcome of the reaction, yielding either any desired CaSO 4 phase in pure state or binary mixtures with predefined compositions. This concept provides full control over phase selection in CaSO 4 mineralization and may allow for the targeted fabrication of corresponding materials for use in various areas.