Intrinsic 3D Prestressing: A New Route for Increasing Strength and Improving Toughness of Hybrid Inorganic Biocements

Cement is the most consumed resource and is the most widely used material globally. The ability to extrinsically prestress cementitious materials with tendons usually made from steel allows the creation of high-strength bridges and floors from this otherwise brittle material. Here, a dual setting cement system based on the combination of hydraulic cement powder with an aqueous silk fibroin solution that intrinsically generates a 3D prestressing during setting, dramatically toughening the cement to the point it can be cut with scissors, is reported. Changes of both ionic concentration and pH during cement setting are shown to create an interpenetrating silk fibroin inorganic composite with the combined properties of the elastic polymer and the rigid cement. These hybrid cements are self-densifying and show typical ductile fracture behavior when dry and a high elasticity under wet conditions with mechanical properties (bending and compressive strength) nearly an order of magnitude higher than the fibroin-free cement reference.