Growing Nanocrystalline Graphene on Aggregates for Conductive and Strong Smart Cement Composites

Highly conductive concrete/mortar has been long pursued to realize structural health monitoring in the development of smart-cement-based facilities. However, it remains challenging to significantly increase the electrical conductivity of concrete/mortar without lowering the compressive strength and flowability. Here, nanocrystalline-graphene-coated aggregates (termed Gr@AGs) are synthesized to break this conductivity-strength tradeoff. Admixing Gr@AGs with cement enables the construction of a conductive network of graphene that simultaneously strengthens the interfacial transition zone between aggregates and paste. As a result, high conductivity and improved mechanical properties have been simultaneously realized in Gr@AGs-based smart mortars. The significant positive effects of Gr@AGs are further enhanced by combining them with a low percentage of carbon fiber. Typically, the 28-day compressive/flexural strength of the optimized mortar increases by 12.2%/19.4%, with the electrical resistivity reduced by over 3 orders of magnitude from ∼4.6 × 10⁵ to 182 Ω cm. On this basis, we demonstrate high-sensitivity cement-based piezoresistive sensors with a fractional change in resistivity as high as ∼25%, which is more than 1 order of magnitude higher than those reported in comparable systems. This study provides a solution to the critical issues in developing smart cementitious composites by taking full advantage of graphene's properties.