This study presents a hierarchical conductive-network strategy to overcome the performance trade-off in cement structural supercapacitors (CSSCs). By incorporating one-dimensional carbon nanotubes (CNTs) and two-dimensional graphene oxide (GO) into Portland cement, we simultaneously enhance its electrochemical and mechanical properties. The approach exploits the complementary roles of the two nanomaterials: CNTs establish a three-dimensional percolation network that facilitates electron transport, while GO promotes formation of a denser calcium silicate hydrate (C-S-H) gel and refines the pore structure by complexing with calcium ions, thereby improving ionic pathways. The k12gc sample attains a specific capacitance of 66.8 F g−1 at 0.1 mA cm−2, a 58.4% rise in conductivity and a 63% reduction in charge-transfer resistance. At the same time, the composite reduces harmful macropores by 27.9% and strengthens the material, with compressive and flexural strengths increasing by 4.8% and 8.3%, respectively. This work establishes a rational design principle based on functional division between CNTs and GO for developing high-performance, multifunctional CSSCs.
Zhang et al. (Mon,) studied this question.