Preparation of Regular Cement Hydration Crystals and Ordered Microstructures by Doping GON and an Investigation into Its Compressive and Flexural Strengths

In this work, we found that by controlling the size of the graphene oxide nanosheets (GON) at 5–140 nm, 5–260 nm and 5–410 nm, respectively, we could prepare regular shaped cement hydration crystals with the shape of nano-needle-like, flower-like, and polyhedron-like crystals, respectively. Together, these crystals formed an ordered structure of cement composites on both the micro and macro levels, and the compressive and flexural strengths of the cement composites obviously increased when compared to the control samples. Our results indicated that the smallest structural unit of regular crystals was the nano-polyhedron-like crystals, which consisted of AFt, AFm, CH, and crystallization C–S–H, and could assemble into regular needle-like crystals, flower-like crystals, and polyhedron-like crystals, as well as an ordered structure on the micro and macro levels. Most of the C-S-H was transferred into a monoclinic system crystals and the remainder played the role of an adhesive in the forming process of regular crystals and structure. The cracks and holes in the cement composites disappeared by the self-repairing effect of the growing hydration crystal. The results indicate that ordered structural cement composites with defect-free structures and high strength can be prepared using GON with a suitable size range.