Nano‐crystalline cellulose,chemical blowing agent,and mold temperature effect on morphological,physical/mechanical properties of polypropylene

Polypropylene (PP)/nano‐crystalline cellulose (NCC) composites and foams were produced through extrusion compounding combined with injection molding. From the samples produced, a complete morphological, physical, and mechanical analysis was performed to study the effect of NCC concentration (0–5wt %), foaming agent content (0 to 2wt %) and mold temperature (30°C and 80°C). NCC was very effective to reduce cell size (42–71%) and increase cell density (5–37 times) of the foams, while slightly increasing the overall density (2–7%). The results showed that NCC addition increased the specific tensile modulus (15–22%), specific tensile strength (1–14%) and specific flexural modulus (13–26%) of PP, but decreased specific impact strength (10–20%) and specific elongation at break (50–96%). © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42845.     

Physicomechanical properties of irradiated SBR latex polymer‐modified cement mortar composites

This study investigated the effect of styrene–butadiene‐rubber (SBR) latex/cement ratio as well as γ‐irradiation dose on physicomechanical properties of cement mortar. Specimens were prepared with a different SBR/cement mass ratio of 2.5, 5, 10, 15, and 20. Two curing methods were used: wet cure and dry cure. The best specimens were irradiated to doses of 10, 30, and 50 kGy. The compressive strength, total porosity, and bulk density were studied. The result indicated that the compressive strength, total porosity, and the bulk densities of the composites decrease with increase in the polymer cement ratios. In addition, it was observed that the compressive strength of irradiated polymer‐modified cement mortar composites was improved with the increase in the γ‐irradiation dose, and the compressive strength of mix‐cured samples was higher than those wet‐cured samples at any irradiation dose. X‐ray diffraction, thermogravimetric analysis, acid attack, and microstructure of SBR‐modified cement mortar were characterized. J. VINYL ADDIT. TECHNOL., 26:144–154, 2020. © 2019 Society of Plastics Engineers     

Mechanical and barrier properties of nanocrystalline cellulose reinforced poly(caprolactone) composites: Effect of gamma radiation

Nanocrystalline cellulose (NCC) reinforced poly(caprolactone) (PCL) composites were prepared by compression molding. The NCC content varied from 2 to 10% by weight. NCC played a significant role in improving the mechanical properties of PCL. The addition of 5 wt % NCC caused a 62% improvement of the tensile strength (TS) value of PCL films. Similarly, tensile modulus (TM) values were also improved by NCC reinforcement but elongation at break (Eb) values decreased montonically with NCC content. The water vapor permeability (WVP) of PCL was 1.51 g·mm/m²·day·kPa, whereas PCL films containing 5 wt % NCC showed a WVP of 1.22 g·mm/m²·day·kPa. The oxygen transmission rate (OTR) and carbon dioxide transmission rate (CO₂TR) of PCL decreased by 19 and 17%, respectively, with 5 wt % NCC incorporation. It was found that the mechanical and barrier properties of both PCL and PCL‐NCC composites further improved with 10 kGy gamma irradiation treatment. The combination of NCC and radiation significantly increased the TS, TM, and Eb (by 156, 123, and 80%, respectively, compared to untreated PCL). The WVP, OTR, and CO₂TR decreased by 25–35% with respect to untreated PCL. The surface and interface morphologies of the PCL‐NCC composites were studied by scanning electron microscopy and suggested homogeneous distribution of NCC within the PCL matrix. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

Utilization of emulsion polymer for preparing bagasse fibers polymer–cement composites

Sugarcane‐bagasse fiber–polymer cement composites were prepared using three lattices namely, styrene butadiene, vinyl ester, and styrene acrylic. The lattices percentages ranged between 3 and 21% from the weight of the mixture. The pressed samples were irradiated at different irradiation doses by using electron beam (EB) accelerator. Comparative studies have been made for physicomechanical properties of unirradiated and irradiated samples. The results indicated that the flexural strength, modulus of elasticity, and impact toughness of the composites increase with the increasing polymer content up to 9.9 and 15% of styrene butadiene, vinyl ester, and acrylic styrene, and then decrease. It was also observed that the maximum values of flexural strength and modulus of elasticity obtained at EB‐irradiation dose 45, 40, and 25 kGy for styrene butadiene, acrylic ester, and vinyl ester, respectively. The impact strength of the composites did not significantly improve above 10 kGy. The average values of hardness of irradiated composites were higher than that those of unirradiated and control composites. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Effects of styrene–acrylic emulsion on bond performance and interface microstructure of repair mortar of ternary cementitious system

This study investigates the effects of styrene–acrylic emulsion (SAE) as a modifier and interfacial agent on the interfacial bond performance of ordinary Portland cement–aluminate cement–gypsum (PAG) repair mortar. The hydration products and interfacial microstructure are analyzed via x-ray diffraction (XRD), x-ray photoelectron spectroscopy (XPS), Fourier-transform infrared (FTIR) spectroscopy, and scanning electron microscopy (SEM). The results demonstrate that the addition of SAE can effectively enhance the tensile bond strength and flexural bond strength of the PAG repair mortar, and the optimal addition amount of SAE is 10 wt%. The tensile and flexural bond strengths of the PAG repair mortar with SAE interfacial agent at 40% concentration are 1.38 and 1.34 times than those of the mortar without the interfacial agent, respectively. XPS and FTIR analyses reveal that the carboxyl groups in SAE and Ca²⁺ generated from cement hydration form Ca²⁺–carboxyl complexes. The SEM and XRD analyses indicate that SAE can alter the distribution and size of crystals at the bond interface and considerably reduce the thickness of the bond interface; however, SAE cannot change the type of hydration products at the bond interface.     

Mechanical,thermal, and transport properties of nitrile rubber–nanocalcium carbonate composites

The article describes the properties of acrylonitrile butadiene copolymer (NBR)–nanocalcium carbonate (NCC) nanocomposites prepared by a two‐step method. The amount of NCC was varied from 2 phr to 10 phr. Cure characteristics, mechanical properties, dynamic mechanical properties, thermal behavior, and transport properties of NBR–NCC composites were evaluated. For preparing NBR nanocomposites, a master batch of NBR and NCC was initially made using internal mixer. Neat NBR and the NBR–NCC masterbatch was compounded with other compounding ingredients on a two roll mill. NCC activated cure reaction upto 5 phr. The tensile strength increased with the nanofiller content, whereas NBR–NCC containing 7.5 phr exhibited the highest modulus. The storage modulus (E′) increased up to 5 phr NCC loading; the reinforcing effect of NCC was seen in the increase of modulus which was more significant at temperatures above T_g. The effect of nanofiller content and temperature on transport properties was evaluated. The solvent uptake decreased with NCC content. The mechanism of diffusion of solvent through the nanocomposites was found to be Fickian. Transport parameters like diffusion, sorption, and permeation constants were determined and found to decrease with nanofiller content, the minimum value being at 7.5 phr. Thermodynamic constants such as enthalpy and activation energy were also evaluated. The dependence of various properties on NCC was supported by morphological analysis using transmission electron microscopy. © 2012 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Synthesis and physicochemical study of bisphenol‐C‐formaldehyde‐toluene diisocyanate polyurethane–jute and jute–rice husk/wheat husk composites

Bisphenol‐C‐formaldehyde‐toluene‐2,4‐di isocyanate polyurethane (PU) has been synthesized at room temperature and used for the fabrication of jute and jute–rice husk/wheat husk hybrid composites. PU–jute and PU–jute–RH/WH composites were prepared under pressure of 30.4 MPa at room temperature for 8 h, while PU–jute–RH/WH composites were prepared under same pressure at 110°C for 5 h. PU–jute composite has good tensile strength and flexural strength (50–53 MPa), while PU–jute–RH/WH hybrid composites have moderate tensile strength (9–11 MPa) and a fairly good flexural strength (15–31 MPa). Composites possess 1.1–2.2 kV electric strength and 0.94–1.26 × 10¹² ohm cm volume resistivity. Water absorption in PU–jute composite is different in water (9.75%), 10% HCl (12.14%), and 10% NaCl (6.05%). Equilibrium water uptake time in salt environment is observed 96 h, while in pure water and acidic environments it is 192 h. In boiling water equilibrium water content and equilibrium time are found to be 21.7% and 3 h, respectively. Water absorption increased 2.2 times in boiling water, whereas equilibrium time reduced 64 times. Thus, PU–jute composite has excellent hydrolytic stability against boiling water, 10% HCl, and 10% NaCl solutions. Fairly good mechanical and electrical properties and excellent hydrolytic stability of composites signify their usefulness for low cost housing units and in electrical and marine industries. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 101: 2363–2370, 2006     

Preparation and characterization of electrospun PLA/nanocrystalline cellulose‐based composites

Biodegradable nanocomposites of Nanocrystalline Cellulose (NCC) and electrospun poly‐(lactic acid) were prepared via a new mixing technique. Dispersion of hydrophilic NCC in hydrophobic PLA was improved through aqueous mixing and freeze drying of perfectly suspended NCC with PLA nanofibers. Freeze drying produced aerogels with good mechanical integrity. The aerogels were further processed via hot pressing. Resulting composites displayed an improvement in mechanical properties, which was greatest at temperatures below the glass transition temperature of PLA. The optimum compositions were found to be in the 0.5–3% NCC (by weight) range. Experiments performed also showed that due to electrospinning, the crystallinity of the PLA slightly increased and this is accompanied by a decrease in its glass transition temperature. Furthermore, adding NCC to the electrospun PLA matrix did not alter the crystallinity of the final composite. The composites investigated proved their potential to be used in packaging and tissue engineering applications. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 3345–3354, 2013     

Study on mechanical properties of perlite‐filled gamma‐irradiated polypropylene

This study covers the preparation and characterization of perlite‐filled polypropylene (PP). The compositions of 15, 30, and 50 % by weight perlite–PP composites were prepared by melt‐mixing. The PP used in this study was either applied in the virgin form or γ‐irradiated in air at the doses of 10, 25, 50, and 100 kGy to determine the effect of oxidative degradation in composite properties. Furthermore, the active sites containing oxygen produced by γ‐irradiation in PP may provide a possible enhancement by the interfacial interaction between perlite and PP. An initial sharp drop in torque readings during the melt‐mixing of perlite–PP composite preparation indicated an extensive chain scission and degradation by γ‐irradiation. The thermal properties of the composites were characterized by DSC. The ultimate tensile strength and elongation and also impact strength decreased in all composites with γ‐irradiation. Yet, these changes appeared not to be faster than was the change in unfilled PP upon irradiation. Scanning electron microscopy revealed an interfacial adhesion between perlite and irradiated PP while virgin PP did not show any evidence of adhesion. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 81: 2670–2678, 2001     

Reinforcing effect of nanocrystalline cellulose and office waste paper fibers on mechanical and thermal properties of poly (lactic acid) composites

Nanocrystalline cellulose (NCC) was prepared from office waste paper (OWP) by sulfuric acid hydrolysis method in this paper and it was used to prepare a series of poly (lactic acid) PLA/NCC composites by using a dissolution method in solvent N, N-dimethylformamide solution. The results indicated that with the addition of only 3 wt% NCC, the composites exhibited outstanding mechanical property. The tensile, bending and impact properties of the PLA/3NCC composite were improved by 8.2%, 13.1%, and 35.9% than those of pure PLA, respectively. On this basis, office waste paper fibers (OWF) were also used as a physical blended filler to enhance PLA/NCC composites to reduce the preparation cost of PLA composites and the perfect PLA/NCC/OWF sample was easily manufactured by melting–blending and injection molding. According to the crystallization and melting performance table, both NCC and OWF can act as nucleating agent to promote the crystallization properties on composites, while the blends did not have positive effect on thermal stability. Furthermore, the water absorption and degradation properties of PLA composites were also studied. This work not only provided a novel idea for the utilization of office waste paper but also successfully produced environment friendly composites with favorable mechanical properties and crystallization performance.     

Nano‐Engineered Cements with Enhanced Mechanical Performance

This article reports on the effect of liquid‐state mechano‐chemical activation on performance of nano‐engineered cements (NEC). Microstructural characterization of NEC and contribution of activated cement (AC) phase were investigated using dynamic light scattering, X‐ray diffraction, scanning electron microscope, and isothermal conduction calorimetry techniques. The effect of different parameters of liquid‐state activation, such as duration of activation and the composition of the AC is reported. Due to intensive milling and hydration, the AC is composed of up to 25% of nano‐ and submicrometer‐ sized cement grains and products of hydration, mainly, C–S–H and ettringite. Different quantities of AC (at 10%–30% cement replacing levels) were tested in NEC mortars. The compressive strength of NEC based materials with different types and dosages of AC was investigated. Research results demonstrated that proposed “top‐down” approach for production of nano‐sized and submicrometer phases of AC acting as seeds increases the rate of cement hydration and improves the compressive strength of cement‐based composites.     

Effect of surfactant and electron treatment on the electrical and thermal conductivity as well as thermal and mechanical properties of ethylene vinyl acetate/expanded graphite composites

This study presents an investigation of the electrical and thermal conductivities of composites based on an ethylene vinyl acetate (EVA) copolymer matrix and nanostructured expanded graphite (EG). To improve the EG dispersion in EVA, EG sheets were modified by treating them with the anionic surfactant sodium dodecyl sulphate (SDS) in water. The modified SDS‐EG platelets, after being filtered and dried, were melt‐mixed with EVA to prepare the composites. Finally, both EVA/EG and EVA/SDS‐EG composites were subjected to 50 kGy electron beam (EB) irradiation. SEM images confirm that the irradiated EVA/EG samples had improved interfacial adhesion, while the irradiated EVA/SDS‐EG samples showed even better interfacial adhesion. The gel contents of the irradiated samples without and with SDS treatment increased with increase in EG loading. The EVA/EG composites exhibited a sharp transition from an insulator to a conductor at an electrical percolation threshold of 8 wt %, but with SDS‐EG the electrical conductivity was extremely low, showing no percolation up to 10 wt % of filler. The EB irradiation had no influence on electrical conductivity. The thermal conductivity linearly increased with EG content, and this increase was more pronounced in the case of SDS‐EG, but decreased after EB irradiation. The thermal properties were little influenced by EB irradiation, while better polymer–filler interaction and better filler dispersion as a result of SDS treatment, and the EB irradiation initiated formation of a cross‐linked network, had a positive effect on the tensile properties. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42396.     

Titanium Dioxide and Gamma Irradiation Induced Changes in the Structural,Morphology, and Mechanical Behavior of Ethylene Vinyl Acetate Copolymer

Some composites were prepared depending on ethylene vinyl acetate (EVA) copolymer with 18% VA content and titanium dioxide (TiO₂). These composites were prepared in the ratios of 100/0, 90/10, 80/20, 70/30, and 60/40 by melt mixing method. Gamma radiation at differing doses was applied on pure EVA and composites to investigate the impact on modification of composites. Gel percentage and the Charlesby‐Pinner equation were used to confirm crosslinking increases. X‐Ray diffraction measurement (XRD), scanning electron microscope (SEM), and mechanical testing were all used to investigate the varying effects of the different processes on the structure, morphology, and mechanical behavior of EVA. It was observed that the addition of TiO₂ and gamma irradiation both have a significant effect on the structure and, therefore, the composites' surface morphology. Notable changes of the lattice structure were revealed by the XRD results for both unirradiated and irradiated composites, which were also confirmed by examination of the samples' surface morphology. It was found that the presence and amount of TiO₂ along with the irradiation process has a significant influence upon the EVA's mechanical behavior. When compared with the pure EVA, the results demonstrated a significant enhancement in the mechanical parameters of both unirradiated and irradiated composites, except elongation at break. The mechanical results were in line with gel content analysis. The reliability of gamma radiation as an applied method for controlling long‐term properties is clearly demonstrated. J. VINYL ADDIT. TECHNOL., 26:224–235, 2020. © 2019 Society of Plastics Engineers     

Morphology,thermal, and crystallization properties of poly(butylene succinate)‐grafted Nanocrystalline Cellulose by polymerization in situ

The compounds 1,4‐butanediol, succinic anhydride, and nanocellulose (NCC) were used to synthesize poly(butylene succinate)‐grafted Nanocrystalline Cellulose (PBS‐g‐NCC) nanocomposites via polymerization in situ. The resulting structures were examined by transmission electron microscopic (TEM), scanning electron microscope (SEM), ¹H and ¹³C‐nuclear magnetic resonance spectroscopic (NMR), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), and X‐ray diffraction (XRD) analyses. TEM showed the cellulose to be nanoscale and SEM analysis indicated that 3 wt% NCC dispersed well in PBS matrix. ¹H and ¹³C‐NMR analyses indicated the product to possess peaks characteristic of PBS. DSC analysis clearly showed that the NCC increased the PBS crystallinity when 3 wt% NCC was introduced into PBS matrixes by polymerization in situ, compared to pure PBS. TGA illustrated that the thermal stability of PBS‐g‐NCC was better than that of pure PBS, when 3 wt% NCC was added. XRD analysis suggested that 3 wt% NCC improved PBS crystallinity, which was in good agreement with the present DSC results. POLYM. ENG. SCI., 59:928–934, 2019. © 2018 Society of Plastics Engineers     

Effects of fiber‐surface treatment on the properties of hybrid composites prepared from oil palm empty fruit bunch fibers,glass fibers,and recycled polypropylene

In this article, we report the effects of hybridization and fiber‐surface modification on the properties of hybrid composites prepared from recycled polypropylene (RPP), coupling agents, oil palm empty fruit bunch (EFB), and glass fibers through a twin‐screw extruder and an injection‐molding machine. The surface of the EFB fibers was modified with different concentrations (10–15 wt %) and temperatures (60–90°C) of alkali solutions. The structure and morphology of the fibers were observed with the help of Fourier transform infrared spectroscopy and scanning electron microscopy. Different types of composites were fabricated with untreated, alkali‐treated, and heat‐alkali‐treated fibers. Comparative analysis of the mechanical, structural, morphological, and thermal properties of the composites was carried out to reveal the effects of treatment and hybridization. The analysis results reveal that composites prepared from the alkali‐treated (in the presence of heat) fibers show improved mechanical, thermal, and morphological properties with a remarkably reduced water absorption. Additionally, the crystallinity of RPP also increased with the development of biaxial crystals. The improvement of various properties in relation to the structures and morphologies of the composites is discussed. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43049.     

Effect of nanocrystalline cellulose on morphological,thermal, and mechanical properties of Nylon 6 composites

In this study, nanocomposites based on Nylon 6 and nanocrystalline cellulose (NCC) were prepared by melt compounding. Then, morphological, thermal, and mechanical properties were analyzed for NCC content between 0 and 7 wt%. Morphological analyses showed different roughness in fractured surface of neat Nylon and its nanocomposites caused by the presence of NCC. Mechanical results showed that the optimum properties were obtained at 3% NCC which could be related to relatively good NCC dispersion at low concentrations with good Nylon‐NCC bonding. Overall, flexural (41%) and tensile (23%) moduli, as well as tensile strength (11%) were increased up to 3% of NCC. However, elongation at break and impact strength decreased with NCC addition. Finally, density and hardness showed only a small increase of 5 and 3%, respectively. POLYM. COMPOS., 37:1473–1479, 2016. © 2014 Society of Plastics Engineers     

Preparation and thermomechanical properties of nanocrystalline cellulose reinforced poly(lactic acid) nanocomposites

A two‐step process was developed to prepare nanocrystalline cellulose (NCC) reinforced poly(lactic acid) (PLA) nanocomposites using polyethylene glycol (PEG) as a compatibilizer. It was composed of solvent mixing and melt blending. The NCC was well dispersed in the PLA matrix. A network was formed at high NCC‐to‐PEG ratio at which the amount of the PEG was not enough to cover all the surfaces of the NCC. The formation of the network was confirmed by the occurrence of a plateau for the storage modulus at low frequency. The incorporation of the PEG and NCC could improve the crystallinity of the PLA. The elongation at break increased from 11.0% for the neat PLA to 106.0% for the composites including 6 wt % NCC, impact strength was improved from 0.864 to 2.64 kJ m^?2 and tensile strength did not change significantly for the same 6 wt % NCC composites. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 44683.     

Surface modification of nanocrystalline cellulose and its application in natural rubber composites

As a biopolymer with high mechanical strength, nanocellulose was generally considered as a green filler for reinforcing polymer. In this study, nanocrystalline cellulose (NCC) isolated from softwood pulp was successfully modified by cetyltrimethyl ammonium bromide (CTMAB), a cationic surfactant, and the modified nanocrystalline cellulose (m-NCC) was used to reinforce natural rubber (NR). In this composite architecture, it was found that when the filler content was 5 or 10 phr, the surface modification of NCC improved the dispersion state of NCC in NR matrix and the interfacial interaction between NR and NCC. Therefore, the NR/m-NCC composites exhibited outstanding mechanical properties, and its tensile strength, elongation at break and tear strength was increased by 132.8, 20, and 66.1%, respectively, compared to pristine NR composites. Besides, the modified NCC could accelerate the vulcanization and improve wet-skid resistance and aging resistance of NR composites. It is envisioned that the modified NCC has the potential to be generalized to manufacturing other polymer matrix composites strengthened with nanocellulose.     

Synthesis,characterization and electrorheological properties of poly(o‐toluidine)/Zn conducting composites

In this study, the synthesis, characterization, and electrorheological (ER) properties of poly(o‐toluidine)/Zn, (POT/Zn), composites were investigated. Syntheses of the composites were carried out by a chemical method using ammonium persulfate, (NH₄)₂S₂O₈, (APS), as a free radical initiator. The composites were characterized by Fourier transform infrared (FTIR) spectroscopy, electrical conductivity, magnetic susceptibility, particle size measurements, and scanning electron microscopy (SEM). A series of Zn‐containing composites were prepared (0.8–7.6% by mass), and their conductivities were measured to be within the range of 1.7 × 10^?3–5.0 × 10^?2 Scm^?1. Magnetic properties of POT/Zn composites were analyzed by Gouy scale measurements; it was found that their conducting mechanisms are bipolaron. A series of particle size (13, 17, 18, 26, 83 μm) were prepared by ground milling the crude POT/Zn composites. Colloidal suspensions of POT/Zn composites were prepared in silicone oil (SO), at a series of concentrations (10–30%, m/m), and sedimentation stabilities were measured at 25°C. ER measurements showed that the POT/Zn/SO suspension system was ER active. Thus, the effects of solid particle concentration, shear rate, electric field strength, addition of polar promoters, and temperature (25–125°C) onto ER activities of suspensions were investigated. The ER activity of suspensions was increased with increasing particle concentration and electric field strength and decreasing shear rate and showing a non‐Newtonian flow behavior. τ = 1.1 kPa shear stress was reached for POT/Zn (4.1 wt %, Zn) composite under E = 2.0 kV, c = 15 (%, m/m), , and T = 25°C conditions. It was found that the ER activity was slightly decreased with increasing temperature. Further, the addition of polar promoters had no promoting effect on the ER activity of the suspensions and POT/Zn/SO system was classified as dry ER materials. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 103: 1058–1065, 2007     

Identification of the Thermodynamically Stable Fe‐Containing Phase in Aged Cement Pastes

Current developments in cement chemistry increasingly rely on predictive thermodynamic modeling of the phase composition in cementitious composites with the aim of linking the performance of the material with the phase composition of the material. This approach requires identification of the cement phases that form in hydrating cementitious materials using standard techniques, such as X‐ray diffraction (XRD) and thermal analysis (DTA, TGA), but also state‐of‐the‐art synchrotron‐based techniques, in particular for those cases in which the signals of solid solutions overlap in XRD and TGA measurements. In this study, two ordinary Portland cements, with different chemical compositions and subject to different hydration times (~10, ~50 yr), were investigated aiming at identifying the most stable Fe‐containing cement phase in the cement pastes. The Fe‐containing cement phases and their solid solutions with the Al analogues in the complex cement matrix were analyzed with X‐ray absorption spectroscopy, indicating the formation of a mixed Fe–Al siliceous hydrogarnet as the major Fe‐containing phase. The presence of this phase after long hydration periods and upon selective dissolution of the pastes further indicates that, independent of the chemical compositions of cements, formation of the mixed Fe–Al siliceous hydrogarnet is thermodynamically favored in aged pastes, which is supported by published thermodynamic calculations.