Carbonate Polymorphs Research Articles

Review and Recalculation of Growth and Nucleation Kinetics for Calcite, Vaterite and Amorphous Calcium Carbonate

The precipitation of calcium carbonate is well studied in many fields of research and industry. Despite the fact that, or perhaps because of the fact that, it is well studied in many fields, different approaches have been used to describe the kinetics of the precipitation process. The aim of this study was to collect and compare the data available in the literature and find a consistent method to describe the kinetics of growth and nucleation of the various polymorphs of calcium carbonate. Inventory of the available data showed that a significant number of the literature sources were incomplete in providing the required information to recalculate the kinetic constants. Using a unified method, we obtained a unique set of parameters to describe the kinetics for growth for calcite, vaterite and amorphous calcium carbonate (ACC) and nucleation for vaterite and ACC. Recalculation of the kinetic constants demonstrated that calcite confirmed there are two growth mechanisms within one polymorph, namely pure spiral growth and spiral growth mixed with surface nucleation. The spiral growth does not show second-order growth, which is typically attributed to it. Re-evaluation of the available nucleation data confirmed the suggested existence of a second pure ACC polymorph with a solubility product between 10−5.87 and 10−5.51 mol2 kgw−2.

Pilot study to investigate the effect of long-term exposure to high pCO2 on adult cod (Gadus morhua) otolith morphology and calcium carbonate deposition

To date the study of ocean acidification on fish otolith formation has been mainly focused on larval and juvenile stages. In the present pilot study, wild-captured adult Atlantic cod (Gadus morhua) were exposed to two different levels of pCO2, 422µatm (ambient, low pCO2) or 1091µatm (high pCO2), for a period of 30 weeks (from mid-October to early April 2014–2015) in order to study the effects on otolith size, shape and CaCO3 crystallization amongst other biological parameters. We found that otoliths from cod exposed to high pCO2 were slightly smaller (− 3.4% in length; − 3.3% in perimeter), rounder (− 2.9% circularity and + 4% roundness) but heavier (+ 5%) than the low pCO2 group. Interestingly, there were different effects in males and females; for instance, male cods exposed to high pCO2 exhibited significant changes in circularity (− 3%) and roundness (+ 4%) compared to the low pCO2 males, but without significant changes on otolith dimensions, while females exposed to high pCO2 had smaller otoliths as shown for length (− 5.6%), width (− 2%), perimeter (− 3.5%) and area (− 4.8%). Furthermore, while the majority of the otoliths analysed showed normal aragonite deposition, 10% of fish exposed to 1091µatm of pCO2 had an abnormal accretion of calcite, suggesting a shift on calcium carbonate polymorph crystallization in some individuals under high pCO2 conditions. Our preliminary results indicate that high levels of pCO2 in adult Atlantic cod might affect otolith growth in a gender-specific way. Our findings reveal that otoliths from adult cod are affected by ocean acidification, and we believe that the present study will prompt further research into this currently under-explored area.

Cadmium isotopes in Bahamas platform carbonates: A base for reconstruction of past surface water bioproductivity and their link with chromium isotopes

The distribution of cadmium (Cd) within the oceans strongly suggests that it is used as a nutrient by marine phytoplankton. Biologically induced removal of Cd from modern surface waters is accompanied by an isotopic fractionation leaving surface-waters enriched in isotopically heavy Cd. This first study focusses on tying the Cd isotopic record preserved in modern shallow platform carbonates of the Great Bahama Bank (GBB) to conditions in the upper water column, and provides a base for future studies aiming at reconstructing past bioproductivity levels in ancient ocean/basin surface waters. In addition, we compare δ114Cd values with previously published chromium (Cr) isotope values and link signals of bioproductivity with redox conditions in the surface waters. The GBB core samples yield [Cd] (21–188 μg/kg), which increases with depth alongside changes in carbonate mineralogy related to sediment supply and diagenesis. The δ114Cd values of these carbonates are mainly positively fractionated with an average of 0.11‰ ± 0.17 (2σ; n = 17) relative to the NIST 3108 reference standard. Unlike previously observed for Cr isotopes, there is no control of δ114Cd values by relative abundances of the carbonate polymorphs aragonite and calcite in the studied profile. Likewise, δ114Cd values are not correlated to major and trace element (e.g. Ca, Mg, Mn and Sr) contents. We postulate that the burial and diagenetic processes of carbonate cannot modify the Cd isotope signals. Using the experimental fractionation factor for Cd into calcite (−0.45‰), calculated seawater δ114Cd of +0.56 ± 0.17‰ is in agreement with values for modern North Atlantic Surface Seawater. This study's results suggest that δ114Cd values in carbonates are a reliable tool for reconstruction of bioproductivity levels in past surface seawaters, and open new possibilities in combination with Cr isotopes to link these with past ocean redox.

Sclerites of the soft coral Ovabunda macrospiculata (Xeniidae) are predominantly the metastable CaCO3 polymorph vaterite

Soft corals (Cnidaria, Anthozoa, Octocorallia, Alcyonacea) produce internal sclerites of calcium carbonate previously shown to be composed of calcite, the most stable calcium carbonate polymorph. Here we apply multiple imaging and physical chemistry analyses to extracted and in-vivo sclerites of the abundant Red Sea soft coral, Ovabunda macrospiculata, to detail their mineralogy. We show that this species’ sclerites are comprised predominantly of the less stable calcium carbonate polymorph vaterite (> 95%), with much smaller components of aragonite and calcite. Use of this mineral, which is typically considered to be metastable, by these soft corals has implications for how it is formed as well as how it will persist during the anticipated anthropogenic climate change in the coming decades. This first documentation of vaterite dominating the mineral composition of O. macrospiculata sclerites is likely just the beginning of establishing its presence in other soft corals. Statement of significanceVaterite is typically considered to be a metastable polymorph of calcium carbonate. While calcium carbonate structures formed within the tissues of octocorals (phylum Cnidaria), have previously been reported to be composed of the more stable polymorphs aragonite and calcite, we observed that vaterite dominates the mineralogy of sclerites of Ovabunda macrospiculata from the Red Sea. Based on electron microscopy, Raman spectroscopy, and X-ray diffraction analysis, vaterite appears to be the dominant polymorph in sclerites both in the tissue and after extraction and preservation. Although this is the first documentation of vaterite in soft coral sclerites, it likely will be found in sclerites of other related taxa as well.

Replacement of Calcium Carbonate Polymorphs by Cerussite

Replacement of Calcium Carbonate Polymorphs by Cerussite

Preparation and Mineralogical, Spectroscopic and Granulometric Characterization of a Natural Adsorbent Based on a Mixture of Shells from Mehdia Beaches (Morocco)

During this study, we realized the preparation of an adsorbent based on shellfish taken from different areas of the beach of Mehdia (Morocco), and then we carried out their characterization by quantitative (XRD), qualitative (FTIR), optical (SEM-EDS) and granulometric analyses. The results obtained during this study show the shellfish studied is composed of the main minerals such as aragonite (68%) and calcite (32%) while an absence of vaterite. In addition, it shows that the crystalline structure of these shells is mainly composed of two polymorphs of calcium carbonate, namely calcite (CaCO3 (90.7%)) and aragonite (CaCO3 (43.9%)) of better stability. Moreover, they have shown that these calcium carbonates have an extensive porous structure with a specific surface consisting of a heterogeneous layer characterized by rounded particles and other mineral traces. This allows these carriers be used to as adsorbents applied in the removal of heavy metals from wastewater before discharge into the receiving environment.

Visual Imaging of Benthic Carbonate-Mixed Factories in the Ross Sea Region Marine Protected Area, Antarctica

Marine biogenic skeletal production is the prevalent source of Ca-carbonate in today’s Antarctic seas. Most information, however, derives from the post-mortem legacy of calcifying organisms. Prior imagery and evaluation of Antarctic habitats hosting calcifying benthic organisms are poorly present in the literature, therefore, a Remotely Operated Vehicle survey was carried out in the Ross Sea region Marine Protected Area during the 2013–2014 austral summer. Two video surveys of the seafloor were conducted along transects between 30 and 120 m (Adelie Cove) and 230 and 260 m (Terra Nova Bay “Canyon”), respectively. We quantified the relative abundance of calcifiers vs. non-calcifiers in the macro- and mega-epibenthos. Furthermore, we considered the typology of the carbonate polymorphs represented by the skeletonized organisms. The combined evidence from the two sites reveals the widespread existence of carbonate-mixed factories in the area, with an overwhelming abundance of both low-Mg and (especially) high-Mg calcite calcifiers. Echinoids, serpulids, bryozoans, pectinid bivalves and octocorals prove to be the most abundant animal producers in terms of abundance. The shallower Adelie Cove site also showed evidence of seabed coverage by coralline algae. Our results will help in refining paleoenvironmental analyses since many of the megabenthic calcifiers occur in the Quaternary record of Antarctica. We set a baseline to monitor the future response of these polar biota in a rapidly changing ocean.

Influence of ontogenetic development, temperature, and pCO2 on otolith calcium carbonate polymorph composition in sturgeons

Changes to calcium carbonate (CaCO3) biomineralization in aquatic organisms is among the many predicted effects of climate change. Because otolith (hearing/orientation structures in fish) CaCO3 precipitation and polymorph composition are controlled by genetic and environmental factors, climate change may be predicted to affect the phenotypic plasticity of otoliths. We examined precipitation of otolith polymorphs (aragonite, vaterite, calcite) during early life history in two species of sturgeon, Lake Sturgeon, (Acipenser fulvescens) and White Sturgeon (A. transmontanus), using quantitative X-ray microdiffraction. Both species showed similar fluctuations in otolith polymorphs with a significant shift in the proportions of vaterite and aragonite in sagittal otoliths coinciding with the transition to fully exogenous feeding. We also examined the effect of the environment on otolith morphology and polymorph composition during early life history in Lake Sturgeon larvae reared in varying temperature (16/22 °C) and pCO2 (1000/2500 µatm) environments for 5 months. Fish raised in elevated temperature had significantly increased otolith size and precipitation of large single calcite crystals. Interestingly, pCO2 had no statistically significant effect on size or polymorph composition of otoliths despite blood pH exhibiting a mild alkalosis, which is contrary to what has been observed in several studies on marine fishes. These results suggest climate change may influence otolith polymorph composition during early life history in Lake Sturgeon.

Effect of a Carbon Polymorph (Fullerite, Graphite) on the Phase Composition of Mechanocomposites with Iron

Effect of a Carbon Polymorph (Fullerite, Graphite) on the Phase Composition of Mechanocomposites with Iron

Preparation and characterization of ancient recipe of organic Lime Putty-Evaluation for its suitability in restoration of Padmanabhapuram Palace, India

The study aims at preparation and characterization of six organic lime putty (hydraulic Lime + fermented plant extract) using regionally available plants namely Terminalia Chebula (kadukkai), Rosa Sinensis (hibiscus), Palm jaggery (refined sugar), Xanthorrhoeaceae (aloe vera), and Indigofera Tinctoria (neelamari) as per the methods given in the ancient palm leaf of Padmanabhapuram Palace, India. Advanced analytical techniques like Gas chromatography-mass spectroscopy (GC–MS), UV-Spectrophotometer and carbon dioxide quantification were used to study the fermented plant extracts and Fourier transform-infrared spectroscopy (FT-IR), X-ray Diffraction (XRD), Field emission-scanning electron microscopy (FESEM) to study hydrated phases and microstructure of organic lime putty. GC–MS recorded the phytochemical compounds like fatty acids, traces of proteins, polysaccharides and carbohydrates. Fermented kadukkai and neelamari extracts reported as fatty acid, palm jaggery as carbohydrate, hibiscus as polysaccharide and aloevera rich in all the biomolecules. The detection limit of Quantification:0.013 and limit of detection:0.067 for polysaccharides, 0.026 and 0.088 for unsaturated fatty acids was reported through a U.V spectrophotometer for all the herbs. Aloevera and neelamari fermented extracts recorded the CO2 release around 96,000 and 90,000 ppm on 4th day of fermentation, whereas for other herbs it ranged below the recorded readings. Supply of CO2 has initiated the internal carbonation of the lime putty and precipitation of calcite in three different forms aragonite, calcite and vaterite minerals. The addition of organics resulted in high-intensity portlandite peaks and calcium carbonate polymorphs as reported in XRD graphs in agreement with FT-IR analysis. FESEM morphology validated the early formation of carbonate polymorphs, and EDX. has shown that kadukkai lime putty, jaggery lime putty and reference lime putty. mixes have calcium around 35–45%. From the overall results, 3% addition of eco-friendly biopolymers has altered the properties like setting time, water repellency and higher carbonation rate, which is the main reason behind longevity of the structure.

Crystallization of vaterite and aragonite on chitin whiskers

The need for the possibility of producing calcium carbonate crystals by the evaporation method within five minutes and the growth of different calcium carbonate polymorphs on chitin whiskers within the same time frame at room temperature necessitated these report. Chitin whiskers (CHWs) were used as insoluble substrates, while poly (acrylic) acid (PAA) is used as soluble additive. The crystals were grown in chitin whiskers, Poly (acrylic) acid and CHW/PAA composites. The volume fractions for aragonite, vaterite, and calcite are 0.10, 0.25, and 0.65, respectively, in the absence of chitin whiskers or Poly (acrylic) acid. Calcite and aragonite volume fractions decrease in favour of vaterite when PAA and or CHWs were added. SEM images in the absence of CHWs and PAA shows rhombohedral calcites that display steady and step like plane appearances with an average edge of between 1.3 and 1.4 μm. In the presence of only CHWs, the SEM images show a mixture of ellipsoidal and spherical shape vaterites. The spherical vaterites have smooth, rough, and some irregular surfaces. Rod-like aragonite polymorphs were seen when only PAA was used as the template. In the presence of both PAA and CHWs, the rhombohedral shape showed roughness with irregular faces.
 Keywords: Chitin whisker, Calcium carbonate, Calcium, vaterite aragonite, Polymorph, Mole fraction

Carbonation rate and microstructural alterations of class G cement under geological storage conditions

Cementitious grouts are a vital component for the economically-viable implementation of the geological storage of CO2 in providing an engineered long-term seal. In this study a class G cement was carbonated at 80 bar, at either 60 °C or 120 °C, whilst immersed in a synthetic brine for durations of up to 5 months. X-ray computed tomography was used to evaluate the advancement of carbonation depth, whilst SEM/EDXA and XRD were used to characterise microstructural alteration of the cement phases. The microstructure of the ‘main carbonation front’ was found to be representative of the governing reactive transport mechanism. An ill-defined ‘main carbonation front’ during carbonation at 80 bar/60 °C showed a carbonation mechanism controlled by the rate or precipitation/dissolution reactions; diffusion in that case was not the controlling factor. The faster local supersaturation conditions in the pores at 60 °C (with respect to Ca2+ and HCO3−) created a dynamic system of aragonite precipitation from the carbonated to the inner regions of the cement. At 80 bar/120 °C a clearly defined ‘main carbonation front’ with higher compositional density than at 60 °C, was correlated with the fast reactions and diffusion limited evolution of the ‘main carbonation front’. Calcite, as the main result of those fast reactions at 120 °C, filled ubiquitously previously unmineralized voids, creating a system less prone to compositional alterations by chemical changes due to the CO2 plume. This study showed, that the formation of calcium carbonate polymorphs depends on the kinetics of carbonation reactions for a class G cement that is determined by temperature and time. The findings of the current paper can be further used for the understanding of reaction processes within the cements of the CO2 injection wells and assess their long-term chemical stability.

Fluorine incorporation into calcite, aragonite and vaterite CaCO3: Computational chemistry insights and geochemistry implications

The abundant occurrence of calcium carbonate minerals in marine sediments and their high fluorine content suggests that fluorine is a good candidate for reconstructing paleoceanographic parameters. However, the potential of fluorine as a paleoproxy had hardly been explored, and fundamental insights into the behaviour of fluorine in biogenic carbonates and marine sediments is required. A first-principles modelling approach is used here to analyse the incorporation mechanisms of fluorine into crystalline calcium carbonates. We compute F incorporation into the CaCO3 lattice via a number of mechanisms, but concentrate on comparison of the energetics of the two easiest substitution mechanisms: replacing one oxygen atom within the carbonate group to form a (CO2F)− group as against a substitution involving replacement of the CO3 group by two fluorine ions to form a CaF2 defect. These incorporation mechanisms are fundamentally different from that of iodine into calcium carbonates, where a carbon atom is replaced. Our simulations suggest that the substitution of CO32- by F22- is the most favoured and that fluorine is preferentially incorporated into the three naturally-occurring polymorphs of calcium carbonate in the order vaterite ⪆ aragonite ≫ calcite. These results explain the previously-reported preponderance of fluorine in aragonite corals, and lend support to the use of F/Ca as a proxy for ocean pCO2.

Patterns of Element Incorporation in Calcium Carbonate Biominerals Recapitulate Phylogeny for a Diverse Range of Marine Calcifiers.

Elemental ratios in biogenic marine calcium carbonates are widely used in geobiology, environmental science, and paleoenvironmental reconstructions. It is generally accepted that the elemental abundance of biogenic marine carbonates reflects a combination of the abundance of that ion in seawater, the physical properties of seawater, the mineralogy of the biomineral, and the pathways and mechanisms of biomineralization. Here we report measurements of a suite of nine elemental ratios (Li/Ca, B/Ca, Na/Ca, Mg/Ca, Zn/Ca, Sr/Ca, Cd/Ca, Ba/Ca, and U/Ca) in 18 species of benthic marine invertebrates spanning a range of biogenic carbonate polymorph mineralogies (low-Mg calcite, high-Mg calcite, aragonite, mixed mineralogy) and of phyla (including Mollusca, Echinodermata, Arthropoda, Annelida, Cnidaria, Chlorophyta, and Rhodophyta) cultured at a single temperature (25°C) and a range of pCO2 treatments (ca. 409, 606, 903, and 2856 ppm). This dataset was used to explore various controls over elemental partitioning in biogenic marine carbonates, including species-level and biomineralization-pathway-level controls, the influence of internal pH regulation compared to external pH changes, and biocalcification responses to changes in seawater carbonate chemistry. The dataset also enables exploration of broad scale phylogenetic patterns of elemental partitioning across calcifying species, exhibiting high phylogenetic signals estimated from both uni- and multivariate analyses of the elemental ratio data (univariate: λ = 0-0.889; multivariate: λ = 0.895-0.99). Comparing partial R 2 values returned from non-phylogenetic and phylogenetic regression analyses echo the importance of and show that phylogeny explains the elemental ratio data 1.4-59 times better than mineralogy in five out of nine of the elements analyzed. Therefore, the strong associations between biomineral elemental chemistry and species relatedness suggests mechanistic controls over element incorporation rooted in the evolution of biomineralization mechanisms.

Effect of Extended Carbonation Curing on the Properties of γ-C2S Compacts and Its Implications on the Multi-Step Reaction Mechanism

Accelerated carbonation of the cement-based materials has attracted worldwide attention due to the advantages of rapid strength gain and CO₂ sequestration. This work was designed to investigate the mechanism of γ-C₂S compacts under extended carbonation curing to further develop the accelerated carbonation technology. Based on the variation of the mechanical properties, microstructure, and the phase assemblages through the extended carbonation, a multi-step reaction mechanism is proposed in this work. The process can be divided into three stages: phase-boundary-controlled stage; product layer CO₂ diffusion-controlled stage; and CO₂ diffusion and calcium ion dissolution-controlled stage. Correlation between the calcium carbonate polymorph and the controlling factors is also investigated, in which the high calcium ion concentration is beneficial to the formation of calcite. Meanwhile, the stepwise pressurization curing regime based on the multi-steps is proposed to increase the strength obviously, which further verifies the mechanism of multi-step reactions.

Transformation of Calcium Carbonate Polymorph From Various Type of Shells by Carbonation Methods

The utilization of shells can reduce the accumulation of shell wastes and increase the value of shells to achieve ecological and economic incentives. This study examines the transformation of calcium carbonate polymorph from several types of shells to understand the causes of their characteristics in order to suitable for their use. The types of shells used in this experiment are selected based on consumable and their habitats such as snail shells, crab shells, eggshells, batik mussels shells, and golden conch shells. The prepared shells calcinate at 900 °C, the reaction with hydrochloric acid, and carbonation by flowing CO2 into a stirred reactor to produce precipitated CaCO3. The characteristics of polymorph CaCO3 in the sintering temperature of 30, 50, and 70 ℃ were identified by XRD, FTIR, and SEM morphological. The result is that the polymorphs formed from each shell are different in shape, size, and crystallinity. At the temperature of 70 ℃, the rhombohedral calcite was obtained from snail shells, the cubic calcite was obtained from batik mussel shell, while rhombohedral calcite multilayers obtained (100%) from golden conch shells. The aragonite was obtained from batik mussel shells at 30 and 70 ℃. The pure vaterite (100%) was obtained from snail shells and crab shells at 50 ℃. The characteristic of polymorph formed might be useful as information for more suitable applications, especially as nano-bio materials, optical, or filler

The atomic structure and dynamics at the CaCO3 vaterite-water interface: A classical molecular dynamics study.

Classical molecular and lattice dynamics were applied to explore the structure and dynamics of water on different surfaces of vaterite, the least abundant calcium carbonate polymorph. Surfaces were generated starting from the three possible structural models for vaterite (monoclinic, hexagonal/trigonal, and triclinic) and pre-screened using their surface energies in an implicit solvent. Surfaces with energies lower than 0.55 J/m2 were then run in explicit water. The majority of these surfaces dissolve in less than 100 ns, highlighting the low stability of this phase in abiotic environments. Three stable surfaces were identified; they exhibited only minor structural changes when in contact with explicit water and did not show any tendency to dissolve during 1 µs molecular dynamics simulations. The computed water density profiles show that all these surfaces have two distinct hydration layers. The water residence time at the various calcium sites was computed to be within 0.7 and 20.5 ns, which suggests that specific Ca ions will be more readily available to bind with organic molecules present in solution. This analysis is a step forward in understanding the structure of this complex mineral and its role in biomineralization, as it provides a solid theoretical background to explore its surface chemistry. In particular, this study provides realistic surface models and predicts the effect of water exchange at the surface active sites on the adsorption of other molecules.

A parametric study of accelerated carbonation in alkali-activated slag

Resistance to carbonation is one important attribute that low-CO2 cement alternatives must possess, and is particularly crucial for cement alternatives subjected to aggressive CO2 concentrations such as those used in construction of oil wells and wells for below ground carbon sequestration. Here, a parametric study of alkali-activated slag (AAS) carbonation in aggressive environments has been conducted to examine (i) calcium carbonate polymorphism using X-ray diffraction (XRD) and Fourier-transform infrared (FTIR) spectroscopy, and (ii) the extent of calcium carbonate formation and CO2 adsorption using thermogravimetric analysis (TGA). A range of AASs have been studied by varying the magnesium content of the slag, the activator type (sodium hydroxide and sodium silicate), the activator concentration, and the curing time prior to carbonation. It was uncovered that both (i) magnesium from the slag and (ii) silica from the activating solution are needed to reduce the propensity for the sodium-containing calcium-alumino-silicate-hydrate gel to undergo decalcification.

Establishing the Carbonation Profile with Raman Spectroscopy: Effects of Fly Ash and Ground Granulated Blast Furnace Slag

Establishing the carbonation profile is of great significance to the prediction of the service life of reinforced concrete structures. In our previous work, Raman spectroscopy was shown to be an efficient tool for characterizing calcium carbonate (CaCO3) polymorphs and their profile in plain Portland cement (PC) matrices. However, as supplementary cementitious materials (SCMs), particularly fly ash (FA) and ground granulated blast furnace slag (GGBS), are widely used in concrete, establishing the carbonation profile without considering the possible effects of these SCMs could be of little significance to the real world. This paper, thus, investigated the effects of FA and GGBS on the working capacity and reliability of Raman spectroscopy for establishing the carbonation profile in PC blends containing SCMs. The thermogravimetry (TG) analysis was also conducted to verify the results from Raman spectroscopy. The results show that Raman spectroscopy demonstrated a good capacity for differentiating the variation of CaCO3 contents in FA or GGBS blends. However, the incorporation of FA and GGBS into the PC system caused some adverse effects on the quantification of CaCO3 by Raman spectroscopy, which could be attributed to the darker color and weak scatter nature of FA and the high content of glassy phases in GGBS.

Chemical and mineralogical characteristics of carbonated and uncarbonated cement pastes subjected to high temperatures

The fire-resistance of carbonated concrete under high temperatures is significant due to its direct exposure during an accidental fire. To evaluate the carbonation effect on fire-resistance of concrete, the chemical and mineralogical changes of uncarbonated and carbonated cement pastes subjected to high temperatures were thoroughly investigated in this research by employing micro-measurement methods including thermal-gravimetric analysis (TGA), X-ray diffraction (XRD) and 29Si nuclear magnetic resonance (29Si NMR). Uncarbonated cement paste results showed the decomposition of portlandite at 400 °C with the formation of lime, whilst the depolymerization of C–S–H happened simultaneously to generate monomeric silicon tetrahedron. Above 720 °C, all the C–S–H depolymerized to crystalline C2S. Carbonated cement pastes on the other hand showed that amorphous calcium carbonate and part of vaterite decomposed between the range of 400–600 °C, while the rest of the vaterite and calcite were decomposed at 600–720 °C. The individual content of calcium carbonate polymorph could not be obtained using a TGA curve. Besides, the calcium-modified silicate gel was significantly decomposed at 500 °C and completely depolymerized to crystalline C2S at 950 °C. In summary, carbonated pastes show better resistance to high temperatures with its heat absorption capacity 3.3 times as high as the uncarbonated sample, which delays the temperature development in the inner layer. Therefore, a reasonable carbonation process could help to improve the fire resistance of concrete to some extent.