Silicate Polymerization Research Articles

Structures and transport properties of supercritical SiO2-H2O and NaAlSi3O8-H2O fluids

Abstract Speciation and transport properties of supercritical fluids is critical for understanding their behavior in the Earth’s interior. Here, we report a systematic first principles molecular dynamics simulation study of the structure, speciation, self-diffusivity (D), and viscosity (η) of SiO2 melt, NaAlSi3O8 melt, SiO2-H2O and NaAlSi3O8-H2O fluids at 2000–3500 K with 0–70 wt% H2O. Our calculations show that as the water content increases, the proportion of Q0 species (Qn species, where n is the number of bridging oxygens in an individual Si/Al-O polyhedra) increases while Q4 decreases. The proportions of Q1, Q2, and Q3 species first increase and then decrease with increasing water content. The diffusivity sequence for the supercritical SiO2-H2O fluids is DH >DO >DSi, and for the supercritical NaAlSi3O8-H2O fluids, on the whole, is DNa ≈ DH >DO >DAl ≈ DSi. The viscosities of the two systems decrease drastically at the beginning of the increase in water content, and then decrease slowly. We demonstrate that the exponential decrease in the viscosity of polymerized silicate melt with increasing water content is due to a sharp decrease in the proportion of Q4 species and increase in Si-O-H. The typical structural feature of supercritical fluid is that it contains a large amount of easy-to-flow partially polymerized or depolymerized protonated silicate units, which leads to a low viscosity while being enriched in silicate. This feature provides supercritical fluids the potential to transport elements that are hard to migrate in aqueous fluids or hydrous silicate melts, such as high field strength elements.

Characterization and mechanical properties of one-part geopolymer based on a pure metakaolin

Geopolymers are amorphous silicate polymers that have been extensively studied due to their applications, scientific and technical relevance, and their potential as cement in substitution to Portland. Much of the focus has been in the use of precursors and aggregates that are rarely pure and homogeneous with the use of tailings being very common. The presence of these impurities complicates the interpretation of some spectral methods, mainly infrared spectrometry. Therefore, this research focuses on the use of a nearly pure kaolin main precursor, having only a trace of iron and titanium, along with other almost pure reagents, to achieve an ideal geopolymer. It was possible to produce metakaolinite, resulting in a material with a good size particle (8.24µm) and surface specific area (6.57m2/g). The XRD result shows that the calcination process resulted in 100% of amorphous material. FTIR data revealed the presence of H2O and NaCO3 in the geopolymer. More important, the Si-Al-O various bands located between 1100 and 500cm-1 validate the polymerization reaction effectiveness. SEM-EDS analyses have demonstrated that the reaction with Na2SiO3 and NaOH were nearly complete, concerning the finer metakaolinite particles that comprised the material’s matrix. However, the coarser metakaolinite lamellae, in the 15-35µm range, did not react completely; a thin border layer was enriched with sodium and most of the interior material maintained its Si-Al-O composition. The presence of traces of iron and titanium did not influence in the polymerization reaction. Compressive strength values of the geopolymer have presented good values in the range of 25 to 35 MPa.

Synthesis and characterization of silica-derived, silicate polymers: monovalent (rubidium) /divalent (strontium) system

Silicate polymers containing both monovalent (Rb+) and divalent (Sr2+) ions were synthesized using our new synthesis method. Addition of Sr2+ ions to Rb+ ions made silicates less hygroscopic, as addition of Ca2+ ions to Na+ ions makes Na glass more resistant to water. Water (vapor from atmosphere) works as a plasticizer for the silicate polymer down to the saturation limit. By contrast, an ionic liquid can work as a plasticizer for the silicate glass beyond the limit of water vapor. Plasticization mechanism by an ionic liquid is found to be cation exchange reaction between the silicates and the ionic liquid. Finally, reduction of Tg value is found to be larger when: (1) an IL has better compatibility with ionic groups; (2) the monovalent-ion content of the divalent/monovalent glass is higher; and (3) higher pressure is applied during compression molding. The reasonings of these behaviors are discussed.

<sup>29</sup>Si NMR Investigation of the Effect of Acetic and Oxalic Acids on Portland-Limestone Cement Hydration

The use of carboxylic acids in mix design alters the hydration process of cement, the resulting pore structure of the obtained cement paste, and, consequently, the mechanical properties of concrete. All these changes are directly related to the structure of the calcium silicate hydrate phase. In the present study, the effect of acetic acid and oxalic acid on the hydration of Portland-limestone cement was monitored using solid state 29Si NMR spectroscopy. The results showed that acetic acid facilitated alite and belite hydration, however, the formation of polymerized silicate chains, incorporating Q2p species, begun later than in pure cement paste. Oxalic acid accelerated the polymerization, but slowed down alite and belite hydration. Such behaviors may correspond to decreased porosity (acetic acid addition) and increased strength (oxalic acid addition). Both acids accelerated belite hydration, compared to the pure paste, likely due to an increased acidity of the pore solution. The findings provide structural information about C─S─H phase, to be considered for thaumasite sulfate attack investigations on Portland-limestone cement pastes containing carboxylic acids.

Influence of Al2O3 and SiO2 on the structure and viscosity of iron-compound bearing calcium-aluminosilicate slags

The effect of the addition of Al 2 O 3 on the viscosity of the iron-compound bearing CaO-SiO 2 -Al 2 O 3 -MgO slags with different SiO 2 content (= 30, 40, and 50 wt%) was investigated at high temperatures. The addition of Al 2 O 3 increased the viscosity of iron-compound bearing calcium-aluminosilicate melts. The addition of Al 2 O 3 to the slag at low-SiO 2 content (= 30 wt%) increased the fraction of Fe 2+ at a fixed iron content because Fe 3+ cations prefer to exist as tetrahedral unit, i.e., Fe 3+ [IV], in the melt. On the other hand, the addition of Al 2 O 3 to the slag at high-SiO 2 content (= 50 wt%) increased the fraction of Fe 3+ at a fixed iron content due to the preference of octahedrally coordinated Fe 3+ [VI] in the slag. Although the redox equilibrium reaction of iron in the CaO-SiO 2 -Al 2 O 3 -Fe t O-MgO system was strongly affected by the basicity of the melt, the addition of Al 2 O 3 polymerized silicate networks regardless of the SiO 2 content in the slags. The activation energy for the viscous flow of the slags had a linear correlation with the non-bridged oxygen per tetrahedron (NBO/T) in the aluminosilicate network. Therefore, the viscosity of the iron-compound bearing calcium-aluminosilicate melt was determined by the degree of polymerization within the aluminosilicate networks. • Viscosity-structure relationship of iron-compound bearing calcium-aluminosilicate system was experimentally confirmed. • Al2O3 increased melt viscosity due to polymerization reaction and redox equilibria of iron-compound. • Activation energy of viscous flow was dominantly affected by degree of polymerization of slag.

Determine the coordination of Al and Si of Fe-rich fly ash: The challenge in NMR and how we probe its heterogeneity using X-ray spectromicroscopy

Scanning transmission X-ray microscopy (STXM) coupled with ptychographic imaging at Al and Si K-edge is a new probe to the microscale chemistry of heterogenous materials. Here, the combined techniques are applied to study local coordination environment of Fe-rich fly ash (FA). Ptychographic imaging at Al K- and Si K-edge highlights the fine Al- and Si-rich morphological features, respectively, at 6 nm pixel resolution. STXM visualizes the inter- and intra-particle variations in the silicate polymerization degree and two types of Al coordination environment in FA. The Si K-edge of SiO4 connected with four-fold coordinated Al is higher than SiO4 sharing oxygen with six-fold coordinated Al. The result is consistent with bulk nuclear magnetic resonance spectroscopy measurement of the Fe-rich sample which, however, is sensitive to paramagnetic Fe and time-consuming. We demonstrate that the combined method has great potential in the studies of chemically heterogenous aluminosilicates.

Effects of basalt powder and silica fume on ultra-high-strength cementitious matrix: A comparative study

Understanding the effects of basalt powder on the microstructures and hydration products of ultra-high-strength cementitious matrices (UHSCMs) can contribute to the application of basalt powder in ultra-high-performance concrete. This study assesses the effects of basalt powder and silica fume on cementitious matrices by strength examination, microstructure analysis, and material characterization. The results prove the feasibility of adding basalt powder to UHSCMs. Both basalt powder and silica fume can function as reactive additives for cementitious matrices and improve silicate polymerization in calcium silicate hydrate (C-S-H) gels. The calcium-enrichment of the cementitious matrices containing basalt powder leads to the decalcification of the C-S-H structure, the refinement of the pore structure, and the decrease in the strength of UHSCMs. Moreover, a high-temperature curing procedure can alleviate the above adverse effects of basalt powder on the strength of cementitious matrices. The findings of this study are useful for improving the sustainability of concrete materials with high and ultra-high performance.

Cryogenic freezing: A reliable preservation method of samples for seawater nutrient analysis

AbstractFreezing is a strongly recommended preservation method of samples for seawater nutrient analysis when onboard analysis is not available. Previous studies on the effects of freezing methods have explored issues including freezing period, prefiltration, and freezing speed. In this study, the effects of various freezing and storage temperatures on seawater nutrient analysis were examined using a domestic freezer (−18°C), scientific freezer (−23°C), and cryogenic freezer (−80°C). The results showed no difference between the fresh and frozen samples stored in the cryogenic freezer. The observed differences between samples from the domestic freezer and those from the scientific freezers can be attributed to the freezer auto‐defrost function. Transferring samples between the scientific and cryogenic freezers maintained their condition during freezing and storage when a scientific freezer without an auto‐defrost function was used. Silicate concentrations in frozen samples in the cryogenic freezer were similar to those of the fresh samples, even when the frozen samples were analyzed several hours after thawing. Therefore, a cryogenic freezer is highly recommended for freezing and storing seawater nutrient samples because of its stability and independence from silicate polymer formation.

Strategy for preventing explosive spalling and enhancing material efficiency of lightweight ultra high-performance concrete

The highly dense structure which causes the risk of explosive spalling is one of the major limitations of using ultra high-performance concrete (UHPC). This study developed a lightweight UHPC (L-UHPC) and proposed a strategy to improve its material efficiency and lower the risk of explosive spalling. High-strength hollow glass microspheres and fine lightweight aggregates were jointly used in the UHPC system to achieve light weight and ultra high strength. The L-UHPC was cured at different curing regimes to maximize its material efficiency and prevent its spalling after exposure to high temperature. The experimental results showed that the combination of lightweight materials and dry heat curing was effective in reducing the density (<1800 kg/m3) and enhancing the compressive strength (>150 MPa) of the L-UHPC. By means of minimizing the amount of internal free water, the heat curing approach contributed to avoiding the thermal spalling of the L-UHPC exposed to fire conditions. Microstructural results indicated that the elevated temperature curing promoted the pozzolanic reaction and increased the microhardness of the paste matrix by increasing silicate polymerization of the C-S-H structure. The created voids of the collapsed glass microspheres might accommodate some internal vapor pressure and mitigate the degradation caused by the high temperature exposure. The synergetic effect of the porous materials and the dry heat curing lowered the thermal conductivity and significantly improved the material efficiency of the L-UHPC.

Exploration of Zero-Valent Iron Stabilized Calcium-Silicate-Alginate Beads' Catalytic Activity and Stability for Perchlorate Degradation.

Perchlorate contamination in groundwater poses a serious threat to human health, owing to its interference with thyroid function. The high solubility and poor adsorption of perchlorate ions make perchlorate degradation a necessary technology in groundwater contaminant removal. Here, we demonstrate the perchlorate degradation by employing nano zero-valent iron (nZVI) embedded in biocompatible silica alginate hybrid beads fabricated using calcium chloride (1 wt%) as a crosslinker. The concentration of precursors (sodium alginate, sodium silicate) for bead formation was standardized by evaluating the thermal stability of beads prepared at different sodium silicate and alginate concentrations. Thermal degradation of silica alginate hybrid samples showed a stepwise weight loss during the thermal sweep, indicating different types of reactions that occur during the degradation process. The formation of the silica alginate hybrid structure was confirmed by FT-IR spectroscopy. Scanning electron microscopy (SEM) data revealed the surface morphology of silica alginate hybrid changes by varying sodium silicate and alginate concentrations. nZVI-loaded alginate–silicate polymer bead (nZVI-ASB) exhibited excellent perchlorate degradation efficiency by degrading 20 ppm of perchlorate within 4 h. Our study also showed the perchlorate degradation efficiency of nZVI-ASB is maximum at neutral pH conditions.

Polymeric Structure Evolution Behavior Analysis of Aluminosilicate-Based Smelting Slag

The physical and chemical properties of the CaO–SiO2–Al2O3–MgO slag system depend on structure evolution caused by the synergistic mechanism among the components at high temperature, especially the structural complexity of the anion group. In this study, Si–O, Al–O, and Al–Si–O anion groups were found in the high-temperature slag systems at 1773 K. The [Si2O5]2− (Q3) structural unit of the silicate polymer changed to [Si2O6]4− (Q2), [Si2O7]6− (Q1), and [SiO4]4− (Q0) as the binary basicity (R2) and ω(MgO)/ω(Al2O3) increased, while there was a trend toward a simplified structure. That is, the stability of each structural unit weakened, and the relative content of non-bridging oxygen increased. As a result, the degree of polymerization of slag decreased, and the experimental results of the relative content of non-bridge oxygen can be fitted well with the calculations from the reference documents. At the same time, the number of Si–O–Al structural units gradually decreased. The 27Al-MAS-NMR spectroscopy results showed that the structure of aluminate changed from [AlO4]5− tetrahedral structure to [AlO5]7− pentahedral and [AlO6]9− octahedral structure, and the degree of polymerization of the slag decreased. Comprehensive analysis showed that basicity controlled within 1.2 with the ω(MgO)/ω(Al2O3) ratio; less than 0.55 allows for suitable fluidity and energy-saving ability, which is beneficial for the stable and smooth production of the blast furnace.

Reaction kinetics, microstructure and phase evolution of alkali-activated Si-Mn slag during early age

Alkali-activated material with Si-Mn slag (SiMnS) as precursor is regarded as an efficient way of resource utilization in large-scale and green mode. This study aims to investigate the reaction kinetics, microstructure, and phase evolution of alkali-activated SiMnS during the early age. The reaction kinetics of SiMnS activated by water glass with different modulus was studied by isothermal calorimetry, the phase and the microstructure evolution of reaction products from alkali-activated SiMnS at typical alkali activation reaction (AAR) times (15 min, 30 min, 1 h, 3 h, 12 h, and 24 h) were studied by XRD, FTIR, SEM, BET, and thermogravimetric experiments. Reaction kinetics analysis showed that alkali-activated SiMnS exhibited two main exothermic processes attributing the generation of Si-rich gel (mainly C-S-H) and Al-rich gel (mainly C(N)-A-S-H) respectively. The alkalinity and existence form of polymeric silicate of alkaline activator (AA), which depend on the modulus of AA, determined the intensity of AAR and the characteristics of AAR process respectively. Characterization results of samples indicated that alkali-activated SiMnS could be divided into three steps: formation of Si-rich gel, formation of Al-rich gel, increase of gel polymerization degree, and maturation, respectively. SiMnS can be an alternative raw material in the alkali-activated application.

Interfacial nano-engineering by graphene oxide to enable better utilization of silica fume in cementitious composite

As an industrial by-product, silica fume (SF) has been widely employed as supplementary cementitious material to develop high-performance concrete, and contribute to the sustainability goals of the concrete industry. However, with the typical size in the range of 50–300 nm, SF particles tend to form agglomerations when mixed with water and quickly become covered by a gel-like layer, thus retarding hydration. In this study, SF was coated with graphene oxide (GO) to nano-engineer the interface between SF and cement, aimed to allow better utilization of SF in cementitious composites. We report the concept of a nano/microhybrid via the electrostatic adsorption of negatively charged GO on positively charged modified SF (termed as MSF@GO), which aims to improve the dispersion quality of SF as well as the SF-cement interaction. The addition of 5 wt% modified SF (MSF) and 0.04 wt% GO (by mass of binder) result in a significant improvement of 3-d and 28-d compressive strengths of a cement paste by 56% and 29%, respectively, as compared to the sample incorporating 5 wt% SF. Additionally, the 5MSF@GO paste exhibits a greatly reduced initial sorptivity, by 33% (from 1.56 mm to 1.05 mm), along with the lowest secondary sorptivity. The noticeably higher strengths and lower water transport are primarily attributable to the increased polymerization of calcium silicate hydrates and the refinement of pore structure. This study demonstrates the great potential to improve the utilization efficiency of SF by interfacial nano-engineering with GO nanocoating and provide a new strategy to develop low-carbon cementitious composites for practical applications.

Lignocellulose-Based Superabsorbent Polymer Gel Crosslinked with Magnesium Aluminum Silicate for Highly Removal of Zn (II) from Aqueous Solution.

Lignocellulose (LCE) was ultrasonically treated and intercalated into magnesium aluminum silicate (MOT) clay to prepare a nano-lignocellulose magnesium aluminum silicate polymer gel (nano-LCE-MOT) for the removal of Zn (II) from aqueous solution. The product was characterised using nitrogen adsorption/desorption isotherm measurements, Fourier-transform infrared spectroscopy, scanning electron microscopy and energy-dispersive X-ray spectroscopy. The conditions for the adsorption of Zn (II) on nano-LCE-MOT were screened, and adsorption kinetics and isotherm model analysis were carried out to explore the adsorption mechanism and achieve the optimal adsorption of Zn (II). Optimal adsorption was achieved at an initial Zn (II) concentration of 800 mg/L at 60 °C in 160 min at a pH of 4.52. The adsorption kinetics were explored using a pseudo-second-order model, with the isotherm adsorption equilibrium found to conform to the Langmuir model. The maximum adsorption capacity of the nano-LCE-MOT polymer gel toward Zn (II) is 513.48 mg/g. The materials with adsorbed Zn (II) were desorbed using different media, with HCl found to be the most ideal medium to desorb Zn (II). The optimal desorption of Zn (II) was achieved in 0.08 mol/L HCl solution at 65 °C in 60 min. Under these conditions, Zn (II) was almost completely desorbed from the adsorbents, with the adsorption effect after cycling being slightly different from that of the initial adsorption.

Microstructure and phase assemblage of low-clinker cements during the early stages of carbonation

Blending Portland cement with fly ash or ground granulated blast furnace slag effectively reduces its carbon footprint. However, these materials hydrate more slowly than Portland cement. Therefore, their early-stage behaviour is of interest.Fly ash- and slag-containing cement pastes were cured for 72 h and 28 days before exposure to ambient air (ca. 400 ppm). Changes in carbonation behaviour at 0%, 30% and 60% replacement and w/b ratios (0.40 & 0.57) were studied. All Ca-bearing hydrate phases carbonated, but portlandite effectively buffered carbonation of other phases. Complete portlandite consumption permitted decalcification of the other phases, with substantial removal of Ca and Al from C-S-H and increased silicate polymerisation. When portlandite was present, monosulfoaluminate transformed to hemi- and monocarboaluminate, but complete decalcification only occurred when portlandite was no longer available. Reduced w/b ratios improved carbonation resistance for materials with moderate substitution but couldn't mitigate the effects of high replacement levels.

New sights in early carbonation of calcium silicates: Performance, mechanism and nanostructure

Low calcium minerals were considered as a potential sustainable binder and reported to be reactive to CO2. In this research, the carbonation characteristics of C3S, β-C2S and γ-C2S at early age were investigated in some new sights. The results show that carbonation degree and compressive strength of C3S increased most rapidly in the first 8 h carbonation, then slowed down. After 48 h carbonation, β-C2S and γ-C2S were close to C3S in compressive strength, and apparently higher than C3S in carbonation degree. The crystalline CaCO3 generated by carbonation were mainly calcite and aragonite, while vaterite was observed in β-C2S and γ-C2S within 8 h carbonation. Carbonation curing increased MCL of C-S-H and silicate polymerization. Besides, based on the combination of TG-DTG, XRD and 29Si NMR, the decalcify priority of Ca sites in C-S-H was analyzed. The results indicate that interlayer Ca atoms inside C-S-H participated carbonation first, then the calcium atoms within interlayer and silicate chains of C-S-H would be removed successively.

Thermal, water absorption, and mechanical characterizations of polylactide based nanocomposites: Comparison between sodium and modified montmorillonite as reinforcement materials

AbstractThe research on the polymer silicate layer nanocomposites is currently focusing on maximizing the polymer‐filler interface interaction. This study aimed to elucidate the effect of two different types of montmorillonite (MMT), which were Cloisite sodium (CNa) and Cloisite 10A (C10A), on the thermal, water absorption, and mechanical performances of polylactide (PLA) nanocomposites. Nanocomposites with different clay loadings from 1 to 7 wt% were fabricated by melt intercalation in a twin‐screw extruder. XRD analysis showed an intercalated structure for PLA/C10A at 1 and 3 wt% loadings. From TGA analysis, the initial thermal degradation temperature for PLA/C10A at 1 and 3 wt% showed promising enhancement in thermal stability. DSC results also confirmed that both nanocomposites at clay loadings less than 5 wt% improved thermal properties and crystallinity compared to neat PLA. Storage modulus and tan δ for PLA/C10A shifted towards higher temperature. Water absorption intakes of PLA/C10A at 1 and 3 wt% loadings were reduced by 42% and 39%, respectively. For PLA/C10A at the optimum loading of 3 wt%, tensile strength improved by 21% and strain by 17%. This loading exhibited the finest morphological structure.

Competitive Carboxylate-Silicate Binding at Iron Oxyhydroxide Surfaces.

Dissolved silicate ions in wet and dry soils can determine the fate of organic contaminants via competitive binding. While fundamental surface science studies have advanced knowledge of binding in competitive systems, little is still known about the ranges of solution conditions, the time dependence, and the molecular processes controlling competitive silicate–organic binding on minerals. Here we address these issues by describing the competitive adsorption of dissolved silicate and of phthalic acid (PA), a model carboxylate-bearing organic contaminant, onto goethite, a representative natural iron oxyhydroxide nanomineral. Using surface complexation thermodynamic modeling of batch adsorption data and chemometric analyses of vibrational spectra, we find that silicate concentrations representative of natural waters (50–1000 μM) can displace PA bound at goethite surfaces. Below pH ∼8, where PA binds, every bound Si atom removes ∼0.3 PA molecule by competing with reactive singly coordinated hydroxo groups (−OH) on goethite. Long-term (30 days) reaction time and a high silicate concentration (1000 μM) favored silicate polymer formation, and increased silicate while decreasing PA loadings. The multisite complexation model predicted PA and silicate binding in terms of the competition for −OH groups without involving PA/silicate interactions, and in terms of a lowering of outer-Helmholtz potentials of the goethite surface by these anions. The model predicted that silicate binding lowered loadings of PA species, and whose two carboxylate groups are hydrogen- (HB) and metal-bonded (MB) with goethite. Vibrational spectra of dried samples revealed that the loss of water favored greater proportions of MB over HB species, and these coexisted with predominantly monomeric silicate species. These findings underscored the need to develop models for a wider range of organic contaminants in soils exposed to silicate species and undergoing wet–dry cycles.

Physio-chemical interaction of Ethylene-Vinyl Acetate copolymer on bonding ability in the cementing material used for oil and gas well

Effective bond of cement sheath to casing or formation depends on higher tensile strength and lower young's modulus which are a measure of its ability to withstand deformation under load without parting. This work utilized Ethylene Vinyl Acetate (EVA) redispersible polymer powder as additive in the class G cement to characterize bonding ability. Tensile strength was measured for samples cured at 90 °C for 3 days, whereas compressive strength was measured for samples cured at 120 °C for 1 day and 3 days under atmospheric pressure. The results showed that, with the addition of beyond 10% by weight of cement (BWOC) of polymer, not only tensile strength was improved, but also reduced young's modulus. Addition of EVA additive beyond 10% BWOC showed significant benefit of flexibility in the cement system. FTIR (Fourier Transform Infrared Spectroscopy) indicated that presence of high VA (Vinyl Acetate) has no effect on polymerization of Silicates, which shows it does not hider in the formation of C–S–H phase. Intensity of chemical bond augmented with longer curing time and increased polymer content, as seen in O–H stretching vibration at 3434 cm−1 and from Carboxylate anion at 1571 cm−1 to confirm on hydrolysis. Mercury Intrusion porosimeter (MIP) showed significant reduction in fraction of mesopore sizes within the cement matrix, with the polymer addition.

Morphology-controlled calcium silicate and natural polymer composite materials: synthesis, structure and mechanical properties

ABSTRACT Calcium silicate (CS) composite materials are widely applied in cementitious materials and bone tissue engineering. Extensive studies focused on the traditional organic templates (e.g., surfactant), however, introducing the natural polymers to participate in the synthesis of CS has rarely been studied. In this paper, two kinds of modified natural polymers, i.e., gelatinized sticky rice starch (G-SRS), carboxymethyl chitosan (CMC), were used to participate in the synthesis of CS as a novel green organic templating. The morphology, physicochemical properties of CS composites were investigated by TEM-EDS, FE-SEM, FT-IR, BET, and the mechanical properties of CS compacted pellets were determined by the compressive strength and nanoindentation test. The results show that the particle size, particle shape and pore size of the natural polymer/CS composite were effectively controlled, compared to CS. Specifically, SRS/CS composite exhibited universal spherical CS particle morphology, and the CMC/CS composite exhibited finer particle morphology. Addition of natural polymer increased the compressive strength of CS composite, and 3%SRS/CS with uniform spherical particles structure showed ~62% and ~185% increase in the indentation hardness and elastic modulus, compared to the control CS sample. After the nanoindentation test, the polymer bonding was found in the crack structure of 3%SRS/CS, implying that the SRS/CS composite has the self-healing ability. This work reported the innovative synthesis process, green templating design and techniques, paving the path for designing the bioinspired natural polymer/CS composite structural materials.