Converting industrial waste into a value-added cement material through ambient pressure carbonation.

Converting industrial wastes into value-added building products in an environmental management strategy is a challenging yet vital component of the industrial process. Steel slag (SS), an industrial waste by-product from the steel-making process, is typically disposed of in landfill which consumes land resources and pollutes the environment. This paper explores the possibility of a closed-loop system to convert steel slag into a cement material through carbonation activation, thereby significantly reducing the amount of steel slag waste sent to landfills across Canada. The production of this cementing material can occur next to the steel mill, utilizing steel slag and carbon dioxide collected on-site to fabricate carbon-negative products. To save energy and allow production to be feasible on an industrial scale, ambient pressure (AP) carbonation is developed to reduce carbon emissions while improving their performance. High pressure (HP) carbonation curing and normal hydration (NH) references were also implemented at the same time to justify the application of AP carbonation in reducing CO2 emission. The results of this study found AP carbonation-activated SS compacts have comparable CO2 uptake (about 7.5 tons CO2/100 tons slag) and mechanically compressive strength values as those subjected to HP carbonation, suggesting that AP could be used to replace HP in carbonation curing to ensure a lower energy input. Additionally, AP seemed to possess as effective carbonation as HP. The studies investigated by multiple techniques including X-ray diffractometer (XRD), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR), Raman spectroscopic analysis, and scanning electron microscopy (SEM) aim to identify the microstructure development of carbonated SS paste to assess carbonation results. Developed with life cycle assessment (LCA), environmental impact evaluation shows that AP presents a smaller global warming potential (GWP) value than HP. The comparable CO2 sequestration, satisfactory engineering properties, enhanced microstructure and lesser environmental impact in AP carbonation confirm the feasibility of replacing high pressure with extremely low pressure to cure concrete products. The use of AP carbonation for cement material created using steel slag reduces carbon emissions, energy usage, and natural resource consumption.

Dimensional stability of cement paste and concrete subject to early-age carbonation curing.

Early-age carbonation curing of concrete is receiving more interest in terms of performance improvement and emission reduction. However, the volume change of cement-based products subject to carbonation curing may become a concern because of the potential carbonation shrinkage and its related shrinkage cracking. The purpose of this study was to investigate the dimensional stability of cement paste and concrete subject to the early-age carbonation curing. It was found that the carbonation curing introduced first an initial shrinkage due to water evaporation upon gas injection and then generated an expansion due to CO2 uptake and carbonate precipitation. As carbonation proceeded, the deformation was switched to a secondary shrinkage after expansion. The residual deformation due to carbonation curing was shrinkage in cement paste samples and expansion in concrete samples. This was because the relative expansion due to carbonate precipitation in paste was not large enough to compensate for the shrinkage caused by water loss. However, for concrete samples, the introduction of aggregates reduced the pore spaces in concrete, leading to an expansion owing to the limited precipitation. The results of carbon dioxide uptake, XRD, and SEM analysis confirmed that calcium carbonate formation played a critical role in the relative expansion. The study also showed that cement-based products were more resistant to weathering carbonation after the early-age carbonation curing. After 61-day weathering carbonation exposure, both paste and concrete samples exhibited carbonation shrinkage as a result of carbonation of hydration products. However, the magnitude of shrinkage was much smaller in carbonation curing than in weathering carbonation because of the short period of exposure. Both carbonations did not significantly affect the compressive strength of carbonated products. Carbonation curing likely makes concrete products more dimensionally stable in the long-term service.

Enhancing the Performance of Hemihydrate Phosphogypsum by the Collaborative Effects of Calcium Hydroxide and Carbonation.

Normally, the acidic impurities in hemihydrate phosphogypsum (HPG) must be neutralized when HPG is utilized, and a little amount of calcium hydroxide (CH) is the best choice. In this paper, the effects of excessive CH (5 wt.%, 10 wt.%, 15 wt.% and 20 wt.% of HPG) for carbonation curing on the performance of hardened HPG paste were studied. According to the results of macro tests and microanalyses of XRD, TG, SEM-EDS, MIP and N2 physisorption, it could be verified that CaF2, Ca3(PO4)2 and a large amount of nanoscale CaCO3 crystals were produced as a result of neutralization and carbonation, and the compressive strength and the water resistance of carbonated HPG + CH paste were significantly improved due to the effects of nanoscale CaCO3 crystals on pore refinement and the coverage on the surfaces of gypsum crystals of the hardened paste. Therefore, this study suggests a feasible and green method for recycling HPG/PG, with the collaborative effects of neutralization, performance enhancement and reductions in CO2 emissions.

Effect of curing regime on the immobilization of municipal solid waste incineration fly ash in sustainable cement mortar.

Stabilizing/solidificating municipal solid waste incineration fly ash (MIFA) with cement is a common strategy, and it is critical to study the high-value utilization of MIFA in ordinary Portland cement (OPC) components. With this aim, binary-binding-system mortar was produced by partially replacing OPC (∼50%) with MIFA, and the effects of different curing regimes (steam curing and carbonation curing) on the properties of the cement mortar were studied. The results showed that the setting time of the cement paste was shorten with the increase of MIFA content, and steam curing accelerated the hardening of the mixture. Although the incorporation of MIFA reduced the strength of the mortar, compared to conventional curing method, steam curing and carbonation curing increased the 3-d strength of the mortar. For high-volume MIFA mortars, the CO2-cured samples had the highest long-term strength and lowest permeability. The incorporation of MIFA increased the initial porosity of the mortar, thereby significantly increasing the carbonation degree and crystallinity of the reaction product - CaCO3. Steam curing also further narrowed the difference in the hydration degree between MIFA-modified sample and plain paste, which may be due to the enhanced hydraulic reactivity of MIFA at high temperatures. Although the incorporation of MIFA increased the porosity of the mortar, this waste-derived SCM refined the bulk pore structure and decreased the interconnected porosity. Additionally, the heavy metal leaching contents of MIFA-modified mortars were all below 1%, which meet the requirements of Chinese standards. Compared with standard curing, steam curing and carbonation curing made the early-age and long-term performance of MIFA-modified mortar better, which can promote the efficient application of MIFA in OPC products.

Carbonation Curing on Magnetically Separated Steel Slag for the Preparation of Artificial Reefs.

Magnetic separation is an effective method to recover iron from steel slag. However, the ultra-fine tailings generated from steel slag become a new issue for utilization. The dry separation processes generates steel slag powder, which has hydration activity and can be used as cement filler. However, wet separation processes produce steel slag mud, which has lost its hydration activity and is no longer suitable to be used as a cement filler. This study investigates the potential of magnetically separated steel slag for carbonation curing and the potential use of the carbonated products as an artificial reef. Steel slag powder and steel slag mud were moulded, carbonation-cured and seawater-cured. Various testing methods were used to characterize the macro and micro properties of the materials. The results obtained show that carbonation and hydration collaborated during the carbonation curing process of steel slag powder, while only carbonation happened during the carbonation curing process of steel slag mud. The seawater-curing process of carbonated steel slag powder compact had three stages: C-S-H gel formation, C-S-H gel decomposition and equilibrium, which were in correspondence to the compressive strength of compact increasing, decreasing and unchanged. However, the seawater-curing process of carbonated steel slag mud compact suffered three stages: C-S-H gel decomposition, calcite transfer to vaterite and equilibrium, which made the compressive strength of compact decreased, increased and unchanged. Carbonated steel slags tailings after magnetic separation underwent their lowest compressive strength when seawater-cured for 7 days. The amount of CaO in the carbonation active minerals in the steel slag determined the carbonation consolidation ability of steel slag and durability of the carbonated steel slag compacts. This paper provides a reference for preparation of artificial reefs and marine coagulation materials by the carbonation curing of steel slag.

The carbon uptake and mechanical property of cemented paste backfill carbonation curing for low concentration of CO2.

Large volumes of carbon dioxide are released during mining and ore resource development, and cemented paste backfill (CPB) materials are placed in the mined-out stopes where can be discharged from polluted air containing CO2. The construction of green mines and the goal of achieving carbon neutrality have become an inevitable choice for the mining industry to achieve the harmonious development of rational exploitation of resources and environmental protection. Against this background, to minimize the carbon emissions from the mining industry and promote the efficient utilization of CPB, this study investigated the carbon-uptake characteristics and mechanical property of CPB in underground mined-out stopes with 1.5 % concentration CO2. The results show that the carbonation curing (CC) increased the carbonation rate by nearly 4 times compared to natural curing, while the samples exhibited total carbonation within 28 days. This indicates that CO2 uptake could occur within the CPB. The CO2 was absorbed as calcium carbonate minerals, and each ton of CPB can ideally absorb about 78.4 kg CO2 and treat 2600 m3 of dirty air in the mined-out stopes. The increase in early uniaxial compressive strength (UCS) during CC required a higher cement concentrate, and the CC would retard the development of later compressive strength. Microstructure analysis indicated that the CC refined the pore structure and reduced the porosity of the CPB. It also affected the crystal growth and distribution of hydration and carbonation products, further influencing the difference in strength. In summary, CPB technology can potentially be useful during carbon uptake and may assist in mitigating carbon emissions from the mining industry and promoting environment friendly development.

Mechanical and Microstructural Characteristics of Calcium Sulfoaluminate Cement Exposed to Early-Age Carbonation Curing.

The early-age carbonation curing technique is an effective way to improve the performance of cement-based materials and reduce their carbon footprint. This work investigates the early mechanical properties and microstructure of calcium sulfoaluminate (CSA) cement specimens under early-age carbonation curing, considering five factors: briquetting pressure, water-binder (w/b) ratio, starting point of carbonation curing, carbonation curing time, and carbonation curing pressure. The carbonization process and performance enhancement mechanism of CSA cement are analyzed by mercury intrusion porosimetry (MIP), thermogravimetry and derivative thermogravimetry (TG-DTG) analysis, X-ray diffraction (XRD), and scanning electron microscope (SEM). The results show that early-age carbonation curing can accelerate the hardening speed of CSA cement paste, reduce the cumulative porosity of the cement paste, refine the pore diameter distribution, and make the pore diameter distribution more uniform, thus greatly improving the early compressive strength of the paste. The most favorable w/b ratio for the carbonization reaction of CSA cement paste is between 0.15 and 0.2; the most suitable carbonation curing starting time point is 4 h after initial hydration; the carbonation curing pressure should be between 3 and 4 bar; and the most appropriate time for carbonation curing is between 6 and 12 h.

CO2 Uptake and Physicochemical Properties of Carbonation-Cured Ternary Blend Portland Cement-Metakaolin-Limestone Pastes.

The feasibility of carbonation curing of ternary blend Portland cement-metakaolin-limestone was investigated. Portland cement was substituted by the combination of metakaolin and limestone at levels of 15%, 30%, and 45% by the mass. The ternary blends were cured with four different combinations of ambient and carbonation curing. The mechanical property, CO2 uptake, and mineralogical variations of the ternary blend pastes were investigated by means of compressive strength test, thermogravimetric analysis, and X-ray diffractometry. In addition, volume of permeable voids and sorptivity of the ternary blends were also presented to provide a fundamental idea of the pore characteristics of the blends. The test results showed that the increasing amount of metakaolin and limestone enhanced the CO2 uptake, reaching 20.7% for the sample with a 45% cement replacement level at 27 d of carbonation. Meanwhile, the compressive strength of the samples was reduced up to 65% upon excessive incorporation of metakaolin and limestone. The samples with a replacement level of 15% exhibited a comparable strength and volume of permeable voids to those of the sample without substitution, proving that the ternary blend Portland cement-metakaolin-limestone can be a viable option toward the development of eco-friendly binders.

Effects of CO2 Curing on Alkali-Activated Slag Paste Cured in Different Curing Conditions.

The effect of CO2 curing on alkali-activated slag paste activated by a mixture of sodium hydroxide and sodium silicate solutions is reported in this paper. The paste samples after demolding were cured in three different curing environments as follows: (1) environmental chamber maintained at 85% relative humidity (RH) and 25 °C; (2) 3-bar CO2 pressure vessel; and (3) CO2 chamber maintained at 20% CO2 concentration, 70% RH and 25 °C. The hardened samples were then subjected to compressive strength measurement, X-ray diffraction analysis, and thermogravimetry. All curing conditions used in this study were beneficial for the strength development of the alkali-activated slag paste samples. Among the curing environments, the 20% CO2 chamber was the most effective on compressive strength development; this is attributed to the simultaneous supply of moisture and CO2 within the chamber. The results of X-ray diffraction and thermogravimetry show that the alkali-activated slag cured in the 20% CO2 chamber received a higher amount of calcium silicate hydrate (C-S-H), while calcite formed at an early age was consumed with time. C-S-H was formed by associating the calcite generated by CO2 curing with the silica gel dissolved from alkali-activated slag.

Recycling of waste autoclaved aerated concrete powder in Portland cement by accelerated carbonation.

To recycle waste autoclaved aerated concrete (WAAC) and minimize environmental pollution induced by Portland cement (PC), carbonation curing was performed on cement pastes containing variable replacement levels (0-50%) of waste autoclaved aerated concrete powder. Compressive strength and chloride ion permeability of PC-WAAC specimens were measured and related mechanisms were demonstrated by X-ray diffraction (XRD), 29Si solid-state Nuclear Magnetic Resonance (NMR), thermogravimetry-differential thermal analysis (TG-DTA), mercury intrusion porosimeter (MIP), scanning electron microscope (SEM) and back scattered electron images (BSE) measurements. Results showed that the PC-WAAC specimens presents a higher compressive strength increase than the pure PC specimen after carbonation curing and the optimal dosage of WAAC is 20%. This effect compensates the decreasing strength induced by the incorporation of WAAC. Chloride ion penetration resistance of cement pastes were also improved by carbonation curing due to the refinement of pore structure. Up to 20% of WAAC can be successfully recycled to replace PC without compromising strength and chloride ion permeability. Moreover, around 11.23-19.02% of CO2 by the total binder weight can be captured. Therefore, this technology has a great environmental potential to both recycling of construction waste and capture of greenhouse gas.

Early Age Carbonation Heat and Products of Tricalcium Silicate Paste Subject to Carbon Dioxide Curing.

This paper presents a study on the carbonation reaction heat and products of tricalcium silicate (C3S) paste exposed to carbon dioxide (CO2) for rapid curing. Reaction heat was measured using a retrofitted micro-calorimeter. The highest heat flow of a C3S paste subject to carbonation curing was 200 times higher than that by hydration, and the cumulative heat released by carbonation was three times higher. The compressive strength of a C3S paste carbonated for 2 h and 24 h was 27.5 MPa and 62.9 MPa, respectively. The 24-h carbonation strength had exceeded the hydration strength at 28 days. The CO2 uptake of a C3S paste carbonated for 2 h and 24 h was 17% and 26%, respectively. The X-ray diffraction (XRD), transmission electron microscope coupled with energy dispersive spectrometer (TEM-EDS), and 29Si magic angle spinning⁻nuclear magnetic resonance (29Si MAS-NMR) results showed that the products of a carbonated C3S paste were amorphous silica (SiO2) and calcite crystal. There was no trace of calcium silicate hydrate (C⁻S⁻H) or other polymorphs of calcium carbonate (CaCO3) detected.