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Recently we have reported the direct observation of two-dimensional (2D)Ca-Cl crystals on reduced graphene oxide (rGO) membranes, in which the calciumions are only about monovalent (i.e. ~+1) and metallic rather than insulatingproperties are displayed by those CaCl crystals. Here, we report theexperimental observation and demonstration of the formation of graphene-Ca-Clheterojunction owing to the metallicity of 2D Ca-Cl crystals, unexpectedpiezoelectric effect, room-temperature ferromagnetism, as well as the distincthydrogen storage and release capability of the Ca-Cl crystals in rGO membranes.Theoretical studies show that the formation of those abnormal crystals isattributed to the strong cation-pi interactions of the Ca2+ with the aromaticrings in the graphitic surfaces. Since strong cation-pi interactions also existbetween other metal ions (such as Mg2+, Fe2+, Co2+, Cu2+, Cd2+, Cr2+ and Pb2+)and graphitic surfaces, similar 2D crystals with abnormal valence state of themetal cations and corresponding abnormal properties as well as novelapplications are highly expected. Those findings further show the realisticallypotential applications of such abnormal CaCl material with unusual electronicproperties in designing novel transistors and magnetic devices, hydrogenstorage, catalyzer, high-performance conducting electrodes and sensors, with asize down to atomic scale.

Novel two-dimensional Ca-Cl crystals with metallicity, piezoelectric effect and room-temperature ferromagnetism