Membrane-based photothermal crystallization - a pioneering technology for mining valuable minerals from seawater and brines - exploits self-heating nanostructured interfaces to boost water evaporation, so achieving a controlled supersaturation environment that promotes the nucleation and growth of salts. This work explores, for the first time, the use of two-dimensional graphene thin films (2D-G) and three dimensional vertically orientated graphene sheet arrays (3D-G) as potential photothermal membranes applied to the dehydration of sodium chloride, potassium chloride and magnesium sulfate hypersaline solutions, followed by salt crystallization. A systematic study sheds light on the role of vertical alignment of graphene sheets on the interfacial, light absorption and photothermal characteristics of the membrane, impacting on the water evaporation rate and on the crystal size distribution of the investigated salts. Overall, 3D-G facilitates the crystallization of the salts because of superior light-to-heat conversion leading to a 3-fold improvement of the evaporation rate with respect to 2D-G. The exploitation of sunlight graphene-based interfaces is demonstrated as a potential sustainable solution to aqueous wastes valorization via recovery in solid phase of dissolved salts using renewable solar energy.
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