A very low dosage
of graphene oxide (GO) can enhance the mechanical
durability of cement composites, but the reinforcing enhancement is
highly dependent on the uniform dispersion of graphene in the matrix.
Carboxylic groups at GO nanosheets have a decisive effect on GO aggregation
in an alkaline cement solution because they have a strong complexation
ability with aqueous Ca2+ released by cement hydration
and subsequently crosslinks the adjacent graphene sheets, causing
the immediate coagulation of GO. The available methods of homogeneously
dispersing GO in a cement slurry cannot completely eliminate this
carboxylic-crosslinking-induced GO coagulation. In this study, many
hydroxyl groups were introduced onto the edge and planar nanosheets
to prepare water-soluble hydroxylated graphene (HO-G) by facile ball
milling. The structure of HO-G was thoroughly characterized in detail,
and its dispersion behavior in pure water and Ca(OH)2 was
extensively investigated. These results showed that the prepared HO-G
exhibited good hydrophilicity and excellent colloidal dispersion ability
against high pH and Ca2+ ions compared to GO. The effect
of HO-G on the workability, mechanical strength, and chloride penetrability
of a cement mortar was further studied. At a content of 0.03% by cement
mass, HO-G provided 28.62 and 21.19% enhancements of compressive strength
and 3.85 and 7.89% enhancements of flexural strength at 3 and 28 days,
respectively, while the non-steady-state migration coefficient decreased
by 31.51% compared to the reference mortar. Compared to GO, a lower
dosage of HO-G exhibited a similar reinforcing effect to cement composites
with little adverse impact on the fluidity of the fresh cement slurry.
Moreover, the addition of HO-G could refine the pore structure, accelerate
the hydration process of cement to some degree, and generate more
hydration products so that the structure of the cement mortar was
densified. Considering its environmentally friendly preparation, HO-G,
as a promising reinforcing nanofiller, could provide a new solution
to develop nanoengineered cement composites.