Microstructure of cement paste subject to ambient pressure carbonation curing

This study investigated the microstructure of ordinary Portland cement paste subject to early age ambient pressure carbonation curing in a flexible enclosure. The high-pressure carbonation at 5 bar and the normal hydration were used as references. Both ambient-pressure and high-pressure carbonation was carried out with pure gas (99.9% CO₂) for 12 h. It was found that ambient pressure carbonation could achieve comparable carbon uptake and strength gain as high pressure at both early and late age. Nevertheless, ambient carbonation was more economic and practical for precast products of different sizes and shapes. In order to examine this mechanism, X-ray diffraction (XRD), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR), ²⁹Si nuclear magnetic resonance (NMR), scanning electron microscopy (SEM) and nitrogen adsorption/desorption (NAD) were adopted to characterize the microstructural development after early carbonation curing under both ambient pressure and high pressure. Ambient pressure carbonation reaction took place more on the surface than in the core due to the limited CO₂ diffusion so that the surface layer was more densified. The NAD results showed that ambient pressure performed better than high pressure in terms of reducing the cumulative pore volume and refining the capillary pore size. Ambient pressure could produce well crystalline carbonates as high pressure as deduced by XRD, TGA, FTIR and SEM images. The generation of calcium carbonate and its intermingling effect with hydration products were the main reasons for the strength gain and microstructural development of paste after early carbonation. Besides, SEM images showed that ambient pressure tended to produce calcium carbonates along the surface of C-S-H filling pore structure. As subsequent hydration proceeded, the increase of well crystalline carbonates was seen more in ambient pressure carbonation than high pressure based on TGA. NMR revealed that ambient pressure could enhance the polymerization of silicon in C-S-H promoting the early strength gain and maintain high Ca/Si ratio. © 2021 Elsevier Ltd. All rights reserved.