Calcium Silicate Hydrate Research Articles

Effect of silica fume on the microstructural and mechanical properties of concrete made with 100% recycled aggregates

Recycled concrete aggregate can be utilized in structural concrete in order to reduce the use of natural resources and the harmful impacts of waste concrete on the environment. This present research aimed to assess the effectiveness of using recycled aggregate concrete with the partial replacement of cement by silica fume (SF) to analyze the microstructural and mechanical properties of recycled aggregate concrete (RAC). In this study, recycled stone was used as coarse aggregate. The main variables of the study included the dosage of silica fume that was employed as a partial replacement of ordinary Portland cement (OPC) with four different percentages: 4%, 8%, 12%, and 16% by weight. Five different mixes were prepared, with four mixes created by varying amounts of silica fume, which were designated as RSACSF4, RSACSF8, RSACSF12, and RSACSF16. The other mix was created as a reference mix without silica fume and designated RSACSF0. Slump test was conducted to investigate the workability of concrete mixes. From the test result, a decreasing trend was found after adding more percentage of SF. Compressive and splitting tensile tests were conducted to analyze the mechanical properties of RSAC at 7 and 28 days. The results showed that the addition of SF improved the performance of RSAC at early and later curing ages, and a 12% addition of SF showed the best result. Scanning electron microscopy and X-ray diffraction analysis were performed to explore SF's microstructural performance and effect on RSAC. The results showed that silica fume showed a positive pozzolanic impact, and when combined with calcium hydroxide, it underwent a secondary hydration reaction that boosted the generation of calcium silicate hydrate and improved the parameters of the interface transition zone. X-ray diffraction analysis showed that silica fume and silica fume have similar pattern intensities. Finally, 12% SF is recommended as a partial replacement for cement in RSAC.

Molecular Insights into Adhesion at Interface of Geopolymer Binder and Cement Mortar.

The degradation of concrete and reinforced concrete structures is a significant technical and economic challenge, requiring continuous repair and rehabilitation throughout their service life. Geopolymers (GPs), known for their high mechanical strength, low shrinkage, and durability, are being increasingly considered as alternatives to traditional repair materials. However, there is currently a lack of understanding regarding the interface bond properties between new geopolymer layers and old concrete substrates. In this paper, using advanced computational techniques, including quantum mechanical calculations and stochastic modeling, we explored the adsorption behavior and interaction mechanism of aluminosilicate oligomers with different Si/Al ratios forming the geopolymer gel structure and calcium silicate hydrate as the substrate at the interface bond region. We analyzed the electron density distributions of the highest occupied and lowest unoccupied molecular orbitals, examined the reactivity indices based on electron density functional theory, performed Mulliken charge population analysis, and evaluated global reactivity descriptors for the considered oligomers. The results elucidate the mechanisms of local and global reactivity of the oligomers, the equilibrium low-energy configurations of the oligomer structures adsorbed on the surface of C-(A)-S-H(I) (100), and their adsorption energies. These findings contribute to a better understanding of the adhesion properties of geopolymers and their potential as effective repair materials.

Immobilization capacity of element arsenic in alkali-activated slag-arsenic tailing system during self-healing process

The utilization of alkali-activated slag systems for encapsulating hazardous tailings to produce polymers can effectively reduce the leaching of hazardous elements. Nevertheless, the propensity of these polymers to develop cracks during service poses a risk of secondary release of hazardous elements. For this reason, this study focused on the development of polymer materials using calcium carbide residue (CCR), phosphogypsum (PG), ground granulated blast furnace slag (GGBS), superabsorbent polymers (SAP), and arsenic-containing tailings. The self-healing behavior of the alkali-activated slag system after cracking was analyzed, specifically targeting arsenic immobilization. Additionally, the crack width, crack area, and mechanical properties of the polymers was tested to evaluate their self-healing potential. The results revealed that the main healing products consisted of calcium silicate hydrate (C–S–H), ettringite (AFt), and calcite. These products covered the inner surfaces of the cracks, resulting in a reduction by 78.1–95.9% in arsenic leaching concentration after healing for 56 days. The incorporation of PG led to increased generation of AFt and facilitated secondary hydration reactions for self-healing. This enhanced crack closure and promoted strength recovery while simultaneously improving the pore structure of the crack walls. As a result, the leaching of arsenic from the cracked polymer was effectively inhibited. The mechanism of arsenic immobilization by polymers during self-healing process was as follows: i) adsorption of AsO43− by C–S–H; ii) ion exchange of AFt with AsO43−; iii) physical encapsulation of mixed products including C–S–H, AFt, calcite, and swollen SAP.

Feasibility of adding calcium hydroxide to FETNS–OPC: working performance, mechanical properties and reaction mechanism

To solve the problem of low early-phase reactivity of ferrous extraction tailings of nickel slag (FETNS), the effects of calcium hydroxide (Ca(OH)2) as an alkali activator on the working performance, mechanical properties and hydration products of FETNS–ordinary Portland cement (OPC) composite cementitious systems were studied. The addition of calcium hydroxide was found to shorten the initial setting time by about 40% and the final setting time by about 20%. The compressive strength at 3, 7, 28 and 60 days was increased by 51.95%, 45.27%, 8.53% and 8.9%, respectively, with the addition of calcium hydroxide. Microstructural assessment (by scanning electron microscopy, X-ray diffraction, simultaneous thermal analysis, nitrogen adsorption test and low-field nuclear magnetic resonance analysis) showed that the incorporation of calcium hydroxide increased the reaction degree of the FETNS–OPC system, and more calcium silicate hydrate gel and ettringite were generated to fill internal pores, thus improving the compactness of the matrix. In summary, the incorporation of calcium hydroxide stimulated the early-phase reactivity of the composite system, promoted the formation of reaction products and optimised the internal pore structure.

Water dynamics in calcium silicate hydrates probed by inelastic neutron scattering and molecular dynamics simulations

Calcium-silicate-hydrate (C-S-H) is a disordered, nanocrystalline material, acting as a primary binding phase in Portland cement. C-S-H and C-A-S-H (an Al-bearing substitute present in low-CO2 cement) contain thin films of water on solid surfaces and inside nanopores. Water controls multiple chemical and mechanical properties of C-S-H, including drying shrinkage, ion transport, creep, and thermal behavior. Therefore, obtaining a fundamental understanding of its properties is essential. We applied a combination of inelastic incoherent neutron scattering and molecular dynamics simulations to unravel water dynamics in synthetic C-(A)-S-H conditioned at five hydration states (from drier to more hydrated) and with three Ca/Si ratios (0.9, 1, and 1.3). Our results converge towards a picture where the evolution from thin layers of interfacial water to bulk-like capillary water is dampened by the structure of C-(A)-S-H. In particular, the hydrophilic Ca2+ sites organize the distribution of interfacial C-(A)-S-H water.

Study on the micro-rheological properties of fly ash-based cement mortar

Aiming at the shortcomings of poor rheological properties and low strength of tailings filling mortar, solid waste materials such as fly ash, steel slag, and desulfurization ash were introduced to improve the filling mortar. The Response Surface Methodology (RSM) was used to design the test ratios to determine the significance of the effect of fly ash, steel slag and desulphurization ash on the physical properties of the mortar. The rheological characterization law of filling mortar was studied based on macroscopic L-tube test. The mechanism of filling mortar improvement was analyzed by Scanning Electron Microscopy (SEM), and Energy-Dispersive X-ray Spectroscopy (EDS) and other microscopic tests. The results show that the response-factor model fit regression is significant, with the highest model satisfaction at 12 % fly ash dosing, 15 % steel slag dosing, and 10 % desulfurization ash dosing. The self-flowing extension diameter of the mortar is 15.34 cm, and the 3d and 28d strengths are 0.58 MPa and 3.24 MPa, respectively. Fly ash has effectively improved the phenomenon of mortar segregation and precipitation, and the yield stress of mortar is reduced by 35.1∼64.9 % when the dosage is 8∼12 %. The fractal dimension and mortar workability are positively correlated with fly ash admixture. Fly ash incorporation will gradually consume the calcium hydroxide (CH) to generate alumina ferrite (Aft) and calcium silicate hydrate (C-S-H), which reduces mortar porosity and promotes long-term strength growth. The research results not only realized the effective utilization of solid waste resources, but also significantly improved the performance of the filler and ensured the safe production of the mine.

Thermodynamic insights into the degradation of oil well cement by CO2 under geologic sequestration conditions

Geological carbon storage (GCS) is an effective way to reduce CO2 emissions into the atmosphere. The degradation of oil well cement by CO2 poses a risk to the feasibility of GCS. It is critical to understand how the oil well cement degrades. The previous research is mainly experimental. The objective of this paper is to investigate the degradation of the oil well cement by thermodynamic theory in terms of the chemical reaction of individual phase and the phase evolution of the cement-CO2-water system. The results show that hydration products have different degradation resistance. The order of degradation resistance from best to worst is revealed. The thermodynamic equilibrium of the chemical reactions of degradation is affected by temperature and pressure. The higher the temperature and pressure, the less likely a chemical reaction will occur. Temperature tends to affect more than pressure does. The hydration product of the oil well cement is determined by thermodynamic modeling. The hydration products consist of calcium silicate hydrate solid solution (CSHQ), Si-hydrogarnet solid solution (Si-HG), ettringite solid solution (Ettri), portlandite (CH), and OH-hydrotalcite (OH-HT). The hydration products begin to degrade in the following order: CH, CSHQ, Si-HG, Ettri, and OH-HT. The results can be used to improve the degradation resistance of the oil well cement and research new type of degradation resistant cement. The thermodynamic theory is an effective way to investigate the degradation of the oil well cement by CO2 under geologic sequestration conditions.

Enhancement effect of calcium carbide residue and rice husk ash on soft soil: Small-strain property and micro mechanism

The resource utilization of calcium carbide residue (CCR) and rice husk ash (RHA) is helpful to save resources and alleviate environmental pollution. In this research, CCR and RHA were used to modify soft clay, and the resonant column test was conducted to explore its small-strain dynamic characteristics. The micro-mechanism of CCR-RHA modified soft clay (CRSC) was investigated by using scanning electron microscopy, X-ray diffraction and mercury intrusion tests. The findings demonstrated that the dynamic shear modulus of the CRSC increased with the increase of RHA content and confining pressure, but decreased with the increase of shear strain. In contrast, the damping ratio presents the opposite change law. The Hardin-Drnevich (H-D) model was used to fit the dynamic shear modulus/maximum dynamic shear modulus (G/Gmax)-shear strain γ and the damping ratio D-shear strain γ. As confining pressure increased, Gmax increased but Dmax dropped in CRSC specimens with the same RHA content. The changes of the fitted G/Gmax-γ curve could be divided into progressively decrease stage and rapid decrease stage, while the changes of the fitted D-γ curve could be separated into linear stage and slow stage, with the same turning point γ = 10−4. Microscopic tests revealed that the incorporation of CCR and RHA helped to promote the hydration reaction, and the generated hydration products such as calcium silicate hydrate were able to enhance the integrity and compactness of the CRSC. The results of this research putfward solid foundation for the application of CCR-RHA in the modification of soft soil.

Microstructural analysis and densification of ordinary Portland cement mortars incorporated with minimal nano-TiO2: intermixing and surface coating on both fresh and hardened surfaces

The present study investigated the microstructural properties of ordinary Portland cement (OPC)-modified with minimum dosage of nano TiO2 on fresh and hardened cement mortar surfaces and intermixed samples. X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy-dispersive X-ray spectroscopy (EDX) were used to analyze the morphology and hydration products of the OPC specimens doped with nanotitanium (NT).Additionally, XRD coupled with Rietveld refinement was employed to quantify the crystal phases and refine the crystal structure model through the comparison of the calculated diffraction pattern to the measured pattern. Subsequently, crystallographic analysis was conducted to evaluate the crystallographic structure and to confirm the existence of specific atoms and bonds within the crystal structure altered with NT. The findings revealed that the addition of minimal NT resulted in a more compact and denser microstructure, characterized by increased formation of calcium silicate hydrate (CSH) gel and a reduction in calcium hydroxide (CH) crystals.This led to a reduction in the porosity of the hardened coating surface, with similar improvements observed for the fresh coating and intermixed samples compared to those of the control mortar. A decrease in the lattice parameters, accompanied by an increase in the number of atoms, bonds and polyhedra in the crystal structure, led to alterations in the interatomic spacing and contributed to the densification of the cementitious matrix.The findings also showed that NT integration led to a more compact structure with shorter bond distances and smaller polyhedral volumes for the Ti samples than for the control sample. Moreover, compared with the freshly cast and hardened coating samples, the NT-intermixed samples exhibited the shortest Ti–O bond distances and the smallest polyhedral volume. Overall, the analysis presented in this study significantly contributes to the development of novel and environmentally friendly photocatalytic cementitious materials at minimal dosages.

Potential applicability of calcium phosphate modified portland cement paste for geologic sequestration of CO2

In order to increase the integrity of the wellbore which is used to prevent the leakage of supercritical CO2, it is necessary to develop a concrete that is strongly resistant to carbonation. In an environment where the concentration of CO2 is exceptionally high, Ca2+ concentration in portland cement concrete drops significantly due to the rapid consumption of calcium hydroxide, which decreases the stability of the calcium silicate hydrate. In this work, it is hypothesized that if fairly large quantity of the hydration product becomes more thermodynamically stable than calcite, the damage caused by rapid carbonation will certainly be minimized. For this purpose, portland cement system was modified by monocalcium, dicalcium and tricalcium phosphates to produce hydroxyapatite in portland cement paste. According to the experimental results, addition of calcium phosphate produced hydroxyapatite. Among three different calcium phosphates, monocalcium phosphate showed the most significant impact on hydration. It caused faster stiffening and delayed calcium silicate hydration. Although cement pastes modified by calcium phosphates showed less compressive strength than plain cement paste, they showed an excellent durability after exposure to supercritical CO2. It is clear from the results that the potential applicability of calcium phosphate modification in portland cement for geologic sequestration of CO2 was successfully proven.

Evaluating the pozzolanic activity of andesite and calcined marl for high-performance concrete: a valorization of algerian mineral resources

This study evaluates the pozzolanic activity of andesite and calcined marl sourced from Algeria for potential use as supplementary cementitious materials. The research addresses the need for sustainable construction practices by leveraging local mineral resources. The objectives include assessing the pozzolanic properties of these materials and their effects on mortar mixes. The methodology involves collecting samples from specific quarries, crushing and grinding them into fine powders, and calcining the marl at 750°C. The materials were characterized using X-ray diffraction (XRD), X-ray fluorescence (XRF), and scanning electron microscopy (SEM). Pozzolanic activity was evaluated through Frattini and Saturated Lime Tests, followed by mortar mix analyses with varying substitution levels. Results indicated that andesite and calcined marl exhibit significant pozzolanic activity, with andesite showing the highest reactivity. The inclusion of these additives improved the formation of calcium silicate hydrate (C-S-H) and reduced portlandite content, enhancing the durability and mechanical properties of the mortar. The study concludes that these local mineral resources are viable alternatives to conventional cementitious materials, promoting sustainability in the construction industry.

Molecular dynamics study of ion adsorption on C-S-H under temperature influence

The adsorption of water molecules and ions on the surface of hydrated calcium silicate (C-S-H) in Ca(OH)2 and CaSO4 solutions at different temperatures was simulated. The results show that the adsorption of ions on C-S-H increases with increasing temperature. Hydroxide and sulphate ions mainly surround the cations in solution and interfacial adsorption is not apparent. Notably, at different temperatures, the water molecules at the interface gradually move into the solution because the adsorption of calcium ions is more prominent. The research confirms the impact of temperature on the ion adsorption of C-S-H, offering insights into adhesion mechanisms and providing a theoretical foundation for specialty concrete development.

Characterization of washing aggregate sludge waste as a novel supplementary cementitious material: Experimental study and life cycle assessment

Washing aggregate sludge (WAS), a waste collected from aggregate quarries, is examined for its application as a partial substitute of ordinary portland cement (OPC). The raw WAS initially dried, ground, and then subjected to 700 °C and 900 °C. In this study, various paste and mortar mixtures were produced to investigate the pozzolanic property and environmental impacts of raw WAS and treated WAS at a selected temperature of 700 °C. The pozzolanic activity of both raw and treated WAS at 700 °C was verified using several tests, including X-ray diffraction (XRD), Frattini test, strength-based evaluation, and thermal analysis. The calcium-silicate-hydrate (C–S–H), portlandite (Ca(OH)2), calcium silicates (C2S and C3S), and calcite (CaCO3) were identified as major reaction products indicating the participation of raw or treated WAS. While the reduced [CaO] concentration and location below the solubility curve confirmed the pozzolanic activity of both powders, the compressive strengths of blended mortars were also found greater than 75% compared to the reference mortar at all testing ages. Treated WAS demonstrated higher pozzolanic activity than raw WAS due to the reduced formation of Ca(OH)2 revealed by thermal and kinetic analysis at different time periods. Life cycle assessment resulted in the reduced CO2 emissions by the blended mortars containing either raw or treated WAS, which suggest their promising mechanical and environmental benefits.

The effect of temperature on mechanical properties of calcium silicate hydrate enhanced by graphene oxide and graphene via molecular simulation study

With the advancement of the construction industry, there is a growing demand for cement materials with enhanced high-temperature resistance. This study utilizes reactive molecular dynamics to investigate the impact of elevated temperatures on the mechanical properties of graphene cement-based materials and the underlying mechanisms. The findings suggest that graphene nanosheets (GN) and graphene oxide (GO) can stabilize the structure of calcium silicate hydrate (C-S-H). Moreover, high temperatures can disrupt the H-bond network in composite structures, but the addition of GO can mitigate this effect. Additionally, elevated temperatures can influence the strength of relevant chemical bonds within the composite structure, leading to degradation in tensile strength and Young's modulus. Nevertheless, the incorporation of GO can enhance the mechanical properties of C-S-H at high temperatures. Conversely, the effect of GN on reducing the tensile strength of C-S-H is not significant and may even decrease the stiffness of C-S-H.

Kinetic Study and Catalytic Activity of Cr3+ Catalyst Supported on Calcium Silicate Hydrates for VOC Oxidation.

Volatile organic compounds (VOCs) are pollutants that pose significant health and environmental risks, necessitating effective mitigation strategies. Catalytic oxidation emerges as a viable method for converting VOCs into non-toxic end products. This study focuses on synthesizing a catalyst based on calcium silicate hydrates with chromium ions in the CaO-SiO2-Cr(NO3)3-H2O system under hydrothermal conditions and evaluating its thermal stability and catalytic performance. A catalyst with varying concentrations of chromium ions (10, 25, 50, 100 mg/g Cr3+) was synthesized in unstirred suspensions under saturated steam pressure at a temperature of 220 °C. Isothermal curing durations were 8 h, 16 h, and 48 h. Results of X-ray diffraction and atomic absorption spectroscopy showed that hydrothermal synthesis is effective for incorporating up to 100 mg/g Cr3+ into calcium silicate hydrates. The catalyst with Cr3+ ions (50 mg/g) remained stable up to 550 °C, beyond which chromatite was formed. Catalytic oxidation experiments with propanol and propyl acetate revealed that the Cr3+ catalyst supported on calcium silicate hydrates enhances oxygen exchange during the heterogeneous oxidation process. Kinetic calculations indicated that the synthesized catalyst is active, with an activation energy lower than 65 kJ/mol. This study highlights the potential of Cr3+-intercalated calcium silicate hydrates as efficient catalysts for VOC oxidation.

Multi-step nucleation of C-S-H: DFT simulation on silicate oligomerization and Si(Qn) evolution dynamics

Understanding the nucleation processes of calcium-silicate-hydrate (C-S-H) is fundamental to advancing the performance of cement. This study employs Density Functional Theory (DFT) to reveal the initial stages of C-S-H formation by focusing on silicate oligomerization. It examines the progression from monomer silicate species to the precursor formation, containing a range of silicate tetrahedra. Through DFT simulations, free energy changes and barriers of oligomerization reactions up to pentamers are obtained, unveiling an anionic condensation mechanism that establishes the kinetic and thermodynamic profile of this transformation. Observations reveal a dynamic evolution of Si species, with Si(Q3) indicating a transient presence, suggesting an intricate pathway towards the well-established silicate chain structure of C-S-H. This study provides detailed computational insight into the energy barriers, reaction pathways, and the thermodynamics of C-S-H formation, contributing substantial knowledge to the field of cement chemistry and its multi-step nucleation theory.

Nanostructural characterization of surfaces and interfaces of Portland cement mortars using high resolution microscopy

In Portland cement mortars it is of paramount importance to investigate the bond strength between mortar and masonry by means of the study of interfaces and surfaces that make up the system mortar/ceramic block. In this work the aim was to characterize the chemical compositions, microstructures, surfaces and interfaces of mortars applied on ceramic blocks. Therefore, two important characterization tools were used: field-effect gun (FEG) scanning electron microscope (SEM) - FEI Quanta 200 with energy-dispersive (X-ray) spectrometer (EDS) and SEM system with EGF Nanofabrication FIB - FEI Quanta 3D FEG also with an EDS coupled. To date the results obtained from the research show that the characterization of cementitious materials with high resolution SEM is an important tool in the detection and differentiation of hydrated calcium silicates (CSH), calcium hydroxide (Ca(OH)2), ettringite and calcium carbonate by means of morphological, topographical and chemical data, thus providing extremely reliable as well as qualitative data from the structure of cementitious materials.

Nanostructural characterization of surfaces and interfaces of Portland cement mortars using atomic force microscopy

The characterization of Portland cement mortars is very important in the study of the interfaces and surfaces that make up the system mortar/ceramic block. In this sense, scanning electron microscopy and energy-dispersive (X-ray) spectrometer are important tools in investigating the morphology and chemical aspects. However, more detailed topographic information can be necessary in the characterization process. In this work, the aim was to characterize topographically surfaces and interfaces of mortars applied onto ceramic blocks. This has been accomplished by using the atomic force microscope (AFM) – MFP-3D-SA Asylum Research. To date, the results obtained from this research show that the characterization of cementitious materials with the help of AFM has an important contribution in the investigation and differentiation of hydrated calcium silicates (CSH), calcium hydroxide (Ca(OH)2, ettringite and calcium carbonate by providing morphological and microtopographical data, which are extremely important and reliable for the understanding of cementitious materials.

Preparation and Immobilization Mechanism of Red Mud/Steel Slag-Based Geopolymers for Solidifying/Stabilizing Pb-Contaminated Soil.

Pb-contaminated soil poses serious hazards to humans and ecosystems and is in urgent need of remediation. However, the extensive use of traditional curing materials such as ordinary Portland cement (OPC) has negatively impacted global ecology and the climate, so there is a need to explore low-carbon and efficient green cementitious materials for the immobilization of Pb-contaminated soils. A red mud/steel slag-based (RM/SS) geopolymer was designed and the potential use of solidifying/stabilizing heavy metal Pb pollution was studied. The Box-Behnken design (BBD) model was used to design the response surface, and the optimal preparation conditions of RM/SS geopolymer (RSGP) were predicted by software of Design-Expert 8.0.6.1. The microstructure and phase composition of RSGP were studied by X-ray diffractometer, Fourier transform infrared spectrometer, scanning electron microscopy and X-ray photoelectron spectroscopy, and the immobilization mechanism of RSGP to Pb was revealed. The results showed that when the liquid-solid ratio is 0.76, the mass fraction of RM is 79.82% and the modulus of alkali activator is 1.21, the maximum unconfined compressive strength (UCS) of the solidified soil sample is 3.42 MPa and the immobilization efficiency of Pb is 71.95%. The main hydration products of RSGP are calcium aluminum silicate hydrate, calcium silicate hydrate and nekoite, which can fill the cracks in the soil, form dense structures and enhance the UCS of the solidified soil. Pb is mainly removed by lattice immobilization, that is, Pb participates in geopolymerization by replacing Na and Ca to form Si-O-Pb or Al-O-Pb. The remaining part of Pb is physically wrapped in geopolymer and forms Pb(OH)2 precipitate in a high-alkali environment.

Mix and measure II: joint high-energy laboratory powder diffraction and microtomography for cement hydration studies.

Portland cements (PCs) and cement blends are multiphase materials of different fineness, and quantitatively analysing their hydration pathways is very challenging. The dissolution (hydration) of the initial crystalline and amorphous phases must be determined, as well as the formation of labile (such as ettringite), reactive (such as portlandite) and amorphous (such as calcium silicate hydrate gel) components. The microstructural changes with hydration time must also be mapped out. To address this robustly and accurately, an innovative approach is being developed based on in situ measurements of pastes without any sample conditioning. Data are sequentially acquired by Mo Kα1 laboratory X-ray powder diffraction (LXRPD) and microtomography (µCT), where the same volume is scanned with time to reduce variability. Wide capillaries (2 mm in diameter) are key to avoid artefacts, e.g. self-desiccation, and to have excellent particle averaging. This methodology is tested in three cement paste samples: (i) a commercial PC 52.5 R, (ii) a blend of 80 wt% of this PC and 20 wt% quartz, to simulate an addition of supplementary cementitious materials, and (iii) a blend of 80 wt% PC and 20 wt% limestone, to simulate a limestone Portland cement. LXRPD data are acquired at 3 h and 1, 3, 7 and 28 days, and µCT data are collected at 12 h and 1, 3, 7 and 28 days. Later age data can also be easily acquired. In this methodology, the amounts of the crystalline phases are directly obtained from Rietveld analysis and the amorphous phase contents are obtained from mass-balance calculations. From the µCT study, and within the attained spatial resolution, three components (porosity, hydrated products and unhydrated cement particles) are determined. The analyses quantitatively demonstrate the filler effect of quartz and limestone in the hydration of alite and the calcium aluminate phases. Further hydration details are discussed.