Effect of water-to-cement ratio induced hydration on the accelerated carbonation of cement pastes

Recently, the use of accelerated carbonation curing has attracted wide attention as a promising method to reduce carbon dioxide (CO2) emission and improve the mechanical properties of cement-based materials. However, the diffusion mechanism of CO2 in the matrix and the content of hydration products are the key factors that restrict the carbonation reaction rate. To understand the combined behavior of hydration and carbonation reactions, this paper investigates the influence of cement hydration induced by water-to-cement ratio (w/c) (ranging from 0.25 to 0.45) on microstructure and microhardness properties of cement paste. The experimental results demonstrated that carbonation only occurred at the surface layer of cement paste samples and carbonation efficiency was significantly influenced by greater hydration due to higher w/c. The carbonation depth of the sample with 0.45 w/c was about 6 times higher than that of sample with 0.25 w/c after 28 days of CO2 curing. XRD results revealed that calcite-type calcium carbonate is the main carbonation product and consumption of clinker phases (C2S and C3S) during the hydration enhanced the calcite precipitation in the pores of the surface layer. According to FTIR, with increasing w/c, the position of Si-O-Si stretching bond of the carbonated surface changed from Q(2) to Q(3), confirming the formation of amorphous silica-rich gel, along with the appearance of CO32--bonds related to calcite. In overall, the micro-mechanical analysis in this study showed that the carbonation significantly improved the surface microhardness of cement paste samples, while the refinement of capillary pores due to carbonation also decreased the negative impact of large pores formed in the matrix of cement paste prepared with high w/c. (C) 2021 Elsevier Ltd. All rights reserved.