Crystallization behavior and mechanical properties of high strength mica-containing glass-ceramics from granite wastes

The high-strength mica-containing glass-ceramics were prepared from granite wastes by bulk crystallization. The influences of SiO₂/Al₂O₃ molar ratio (S/A = 7.72, 9.62, 12.58, 17.82 and 29.67) on the crystallization behavior, microstructure, mechanical properties and machinability of glass-ceramics were investigated. The results demonstrated that the polymerization degree of the glass network decreased with the S/A ratio increasing, which further caused the decrease in glass transition temperature and crystallization temperatures. The increase in the S/A ratio promoted the precipitation of diopside, hectorite, kalsilite and tainiolite in glass-ceramics when the samples were heated at 750 °C, while inhibiting the precipitation of forsterite. For the glass-ceramics crystallized at 800 and 900 °C, the main crystalline phases transformed from diopside, forsterite, and nepheline to diopside, kalsilite, and tainiolite, with the S/A ratio increasing. As the SiO₂ gradually replaced Al₂O₃, the morphology of crystals changed from lamellar to granular, while the mean size of crystals reduced. The Vickers-Hardness values of glass-ceramics crystallized at 800 and 900 °C ascended with S/A ratio rising, and the values were above 6.30 GPa. The bending strength of most glass-ceramics is stable between 90 and 140 MPa, among which the maximum bending strength is 133.28 ± 14.81 MPa. The fracture toughness of the glass-ceramic crystallized at 800 and 900 °C declined, while that at 700 °C increased with a larger S/A ratio. Glass-ceramics after heat-treated at 900 °C with S/A ratio of 9.62 had the largest fracture toughness of 3.28 ± 0.15 MPa m^1/2. In preliminary tests of machinability, glass-ceramic after heat-treated at 900 °C with S/A ratio of 9.62 showed better results.     

Crystallization-triggered bubbles in glass-ceramics

Bubbles appear sometimes in glass-ceramics and degrade most properties, especially light transmission and fracture strength. In this work, we deduced microstructural conditions that trigger bubble genesis during crystallization of bubble-free glasses. We related bubble formation to some microstructural parameters in two model glass compositions that exhibit internal crystallization: 1.07Na₂O.2CaO.3SiO₂ (1.07N2C3S) and Li₂O.2SiO₂ (L2S). In this way, we constructed bubble maps – experimental diagrams showing a region of bubble nucleation and growth in a crystal size versus crystallinity plot. Both glass-ceramics show bubbles having similar geometry that emerge from crystal/liquid interfaces and propagate into the residual liquid. These diagrams show that holes of the order of the crystal size tend to form in glass-ceramics containing a high-volume fraction crystallized (>50%) and relatively large crystal size (>10 μm). Mass spectroscopy experiments revealed that bubble formation in the 1.07N2C3S system is caused by O₂. We believe the knowledge generated by this work and resulting maps provide a very useful tool for the design of bubble-free glass-ceramics.     

Effect of metastable phase on the crystallization and mechanical properties of MgO-Al2O3-SiO2 glass-ceramics without nucleating agents

Glass-ceramics without nucleating agents usually undergo surface crystallization, which deteriorates the overall performance of the products. In this paper, we evaluated the effects of the metastable MgAl₂Si₃O₁₀ crystalline phase on the crystallization behavior of a MgO–Al₂O₃–SiO₂ (MAS) glass without nucleating agents and mechanical properties of the glass-ceramics obtained. The results demonstrated that the precipitation of metastable MgAl₂Si₃O₁₀ crystallites promotes the crystallization mechanism transformed from surface crystallization into volume crystallization with two-dimensional crystal growth. Furthermore, the grain size of MgAl₂Si₃O₁₀ near the surface of the prepared glass-ceramics was larger than that of MgAl₂Si₃O₁₀ inside, which helps to generate compressive stress and improves its mechanical properties. The glass-ceramics containing metastable MgAl₂Si₃O₁₀ phase exhibited an enhanced hardness in the range of 7.6 GPa–9.5 GPa for indentation loads ranging from 2.94 N to 98 N, and indentation size effect behavior was observed in Vickers hardness tests of both MAS glass and glass-ceramics. The load-independent hardness values for MAS glass and glass-ceramics were reliably evaluated by the modified proportional specimen resistance (MPSR) model of 7.1 GPa and 7.6 GPa, respectively, with a high correlation coefficient of more than 0.9999. This work reveals the unexploited potential of the metastable phase in improving the crystallization ability and mechanical properties of glass-ceramics.     

Effect of ZnO on the crystallization behavior and properties of SiO2–CaO–Al2O3–Fe2O3 glass-ceramics prepared from simulated secondary slag after reduction of copper slag

The feasibility of preparing low-cost glass-ceramics from Zn-containing dust and secondary molten slag generated during the carbothermal reduction of copper slag was investigated. Analytical-grade agents, such as ZnO, Fe₂O₃, SiO₂, CaO, and Al₂O₃, were used to simulate the dust and secondary slag. The effect of ZnO content on the crystallization behavior, structure, and mechanical properties of the glass-ceramics was investigated through X-ray diffraction analysis, scanning electron microscopy-energy dispersive spectrometry, differential scanning calorimetry, Fourier transform infrared spectroscopy, and Raman spectroscopy. The results showed that with increased ZnO content from 0 to 6 wt%, the crystallization activation energy of base glass increased from 386.05 to 425.89 kJ/mol. Meanwhile, the average value of the crystal growth index increased from 1.91 to 4.10, and the highest crystallization rate of the glass-ceramics increased from about 1.44 to 23.11 mm³/min. The increased ZnO in glass-ceramics promoted the precipitation of gehlenite, but inhibit the crystallization of anorthite. When the ZnO content was 6 wt%, the comprehensive properties of the glass-ceramics were better; the flexural strength, microhardness, volume density, water absorption rate, and open porosity were 58.67 MPa, 738.35 HV, 2.92 g/cm³, 0.44% and 1.27%, respectively.     

Tailoring microwave-millimeter-wave dielectric and mechanical properties in CaO–SiO2 glass-ceramics by P2O5 nucleating agent

Glass-ceramics have demonstrated excellent dielectric properties in low-temperature co-fired ceramic (LTCC) technology used in 5G/6G wireless devices. This work studies the mechanical strengths and dielectric properties from microwave to millimeter-wave frequencies in the CaO–SiO₂ glass-ceramics modified via the P₂O₅ as a nucleating agent. The β-wollastonite phase was identified as the primary structure with the preferred ($20\bar{2}$) orientation and parallel plate-like structure in the matrix as P₂O₅ content increases up to 3.5∼5.5 wt%. The P₂O₅ nucleating agent increases degree of long-range crystallization. Elevated mechanical flexural strength of approximately 170 MPa, hardness of ∼720 MPa, and outstanding high-frequency dielectric properties were obtained in the 3.5–5.5 wt% P₂O₅-added CaO–SiO₂ glass-ceramics, due to the enhanced interatomic Si–O bonding in the network. The improved mechanical and dielectric characteristics of the P₂O₅–added CaO–SiO₂ glass-ceramics make the crystallized wollastonite materials for the 5G/6G devices possible.     

Potential utilization of oil sludge incineration bottom ash for glass-ceramics: Crystallization kinetics,properties and toxicological evaluation

The bottom ash (OIBA) generated from the incineration of hazardous oil sludge is classified as a hazardous waste. In this work, the OIBA was applied as raw material to prepare SiO₂-Al₂O₃-CaO system glass-ceramics by melt-sintering with the addition of waste glass wool (GW). The effects of basicity (CaO/SiO₂ ratio, 0.52-1.05) and sintering temperature (900–1050 °C) on the crystallization kinetics, properties, microstructure, leaching concentrations of heavy metals and potential toxicity of glass-ceramics were investigated. The results showed that the crystallization pattern was two-dimensional crystallization, and with the decrease of basicity, the main crystalline phase evolved from gehlenite to diopside. And the glass-ceramics with basicity of 0.88 and sintering temperature of 950 °C exhibited the best comprehensive properties, including density (2.72 g/cm³), water absorption (0.06%), compressive strength (452.45 MPa) and chemical corrosion resistance. In addition, the reduction of heavy metal leaching concentration indicates that produced glass-ceramics showed excellent solidification effect on heavy metals, the low toxicity of glass-ceramics leaching solution to the wheat seeds and Artemia suggests the environmental protection characteristics of OIBA-based glass-ceramics. These findings proved that the glass-ceramics produced by OIBA and GW could be a promising method to dispose hazardous waste with preparing high value-added construction materials.     

The influence of MgO on the crystallization behaviour and properties of SrO-rich phosphosilicate glasses

A series of glass was produced to investigate the effect of MgO/SrO replacement on the crystallization characteristics and properties of phosphosilicate glasses containing high SrO content. The glass samples were synthesized by conventional melting technique based on 5CaO-(40-X)SrO-X MgO– 43SiO₂–7P₂O₅–5CaF₂ (where; X = 10, 20, 30 and 40 mol%). The influence of MgO/SrO replacement on phase assemblages, microcrystalline structures, thermal expansion, and mechanical properties was examined as a function of basic chemical compositions and crystallization parameters. Predominant strontium meta-silicates together with strontium fluoroapatite phases are crystallized from the base glass free of magnesium. The substitution of strontium by magnesium up to 50% led to formation strontium akermanite phase Sr₂MgSi₂O₇ at the expense of SrSiO₃ phase. Whereas the increase of the MgO/SrO of more than 50%, which led to the crystallization of the clino-enstatite MgSiO₃ as a predominant phase. The results show that the α-values of the glass-ceramics are ranged in 94–125 × 10⁻⁶ K⁻¹ over the temperature range (25–500 °C). On the other hand, MgO/SrO replacements led to enhancing the microhardness of the resultant crystalline materials from 4713 Mpa to 6744 Mpa. As a result of the designed glass compositions, promising crystalline phases were obtained as well as good thermal and mechanical properties for the resultant glass-ceramics. Therefore, the designed glass-ceramics can be strongly used as biomaterials especially for bone reconstruction applications.     

Effect of microstructural evolution on the mechanical properties of lepidolite based glass-ceramics

In this paper, effect of microstructural evolution on mechanical property of lepidolite based glass-ceramics of MgO–Al₂O₃–SiO₂–Li₂O–R₂O–F(R=Na, K) system during the crystallization process has been studied. The results show that two distinct regions of strength dependence on grain size are found. The critical values of the flake diameter and aspect ratio of lepidolite are 1.8 and 4.6μm, respectively. The crystallization temperature (T_C) of critical point locates at 1060 °C. When T_C⩽1060 °C, the bending strength increases with heat-treatment temperature ascribing to the randomly oriented and interlocked lepidolite crystallites, which cause crack divert or blunt to limit the further development of the flaw size and increase the surface energy of fracture. While T_C> 1060 °C, the increased boundary shear stress arising from the mismatch of thermal coefficient between the lepidolite crystallite and the residual glass phase results in the decrease of strength.     

Sinterability,microstructure and compressive strength of porous glass-ceramics from metallurgical silicon slag and waste glass

Porous glass-ceramics have been prepared by the direct sintering of powder mixtures of metallurgical silicon slag and waste glass. The thermal behavior of silicon slag was examined by differential thermal analysis and thermogravimetry to clarify the foaming mechanism of porous glass-ceramics. The mass loss of silicon slag below 700 °C was attributed to the oxidation of amorphous carbon from residual metallurgical coke in the silicon slag, and the mass gain above 800 °C to the passive oxidation of silicon carbide. The porosity of sintered glass-ceramics was characterized in terms of the apparent density and pore size. By simply adjusting the content of waste glass and sintering parameters (i.e. temperature, time and heating rate), the apparent density changed from 0.4 g/cm³ to 0.5 g/cm³, and the pore size from 0.7 mm to 1.4 mm. In addition to the existing crystalline phases in the silicon slag, the gehlenite phase appeared in the sintered glass-ceramics. The compressive strength of porous glass-ceramics firstly increased and then decreased with the sintering temperature, reaching a maximal value of 1.8 MPa at 750 °C. The mechanical strength was primarily influenced by the crystallinity of glass-ceramics and the interfaces between the crystalline phases and the glassy matrix. These sintered porous glass-ceramics exhibit superior properties such as light-weight, heat-insulation and sound-absorption, and could found their potential applications in the construction decoration.     

Improved Fracture Behavior of Alumina Microstructural Composites with Highly Textured Compressive Layers

Alumina‐based microstructural composites combining equiaxed and textured layers were fabricated to examine how cracks propagate and the mechanical properties are affected as a function of the residual stress and volume fraction of texture in a multilayer structure. By combining equiaxed and highly textured alumina layers of varying thermal expansion, the embedded textured layers were placed under compressive residual stresses as high as ?670 MPa. Composites with a near constant maximum failure stress of up to 300 MPa were shown to be almost independent of the initial defect size as result of the compressive residual stress in the textured layers. An apparent fracture toughness of up to 10.1 MPa·m^1/2 was obtained for composites with an equiaxed to textured volume ratio of 7.4:1. The high compressive stress in the textured layers arrested cracks, whereas the weak bonding parallel to the basal surfaces of the textured alumina grains caused cracks to deflect within the textured layers. The coupling of these two mechanisms resulted in crack arrest and a maximum work of fracture of ~1200 J/m² or almost 50 times higher than equiaxed alumina. We believe that embedding textured layers having compressive stresses below the surface of multilayer composites represent an important strategy for designing flaw‐tolerant materials with pronounced crack growth resistance and a high work of fracture.     

Sintered sanidine glass-ceramics from industrial wastes

Glass obtained from melting a mixture of industrial wastes (panel glass from dismantled cathode ray tubes, mining residues from feldspar excavation and lime from fume abatement systems of the glass industry) has been employed for the production of sanidine-based glass-ceramics. The glass-ceramics were developed by a sintering treatment with concurrent crystallization, from fine powders (<37 μm), at a relatively low temperature (880 °C). The enhanced nucleating activity of glass surfaces likely promoted the formation of sanidine, hardly found in glass-ceramics, as the main crystal phase. Due to the achieved mechanical properties (bending strength of about 120 MPa, Vickers’ microhardness exceeding 7 GPa) and aesthetic appearance, resulting from a compact and homogeneous microstructure, the obtained sanidine glass-ceramics may find applications as construction materials.     

Micro- and macro-cellular sintered glass-ceramics from wastes

Glass obtained from melting a mixture of industrial wastes (panel glass from dismantled cathode ray tubes, mining residues from feldspar excavation and lime from fume abatement systems of the glass industry) has been employed for manufacturing micro- and macro-cellular sintered glass-ceramics. Micro-cellular glass-ceramics, with a closed porosity, were prepared by the direct foaming of the glass mass, determined by viscous flow sintering of fine powders (<37 μm), due to addition of a SiC-based waste (from the polishing of glass articles). The surface crystallization of glass, upon sintering, limited the porosity (being about 50%), but imparted a remarkable crushing strength to the products (up to about 80 MPa), useful for construction applications. Micro- and macro-cellular glass-ceramics, with an open porosity and very low relative density (from 40 to less than 10%), were prepared by the sintering of fine glass powders mixed with sacrificial poly-methyl methacrylate microbeads or deposited on sacrificial poly-urethane sponges. The crystallization, besides imparting a good mechanical strength, allowed the maintenance of the open-celled morphology, useful for filtering applications.     

Residual stress effect on the fracture toughness of lithium disilicate glass-ceramics

In glass-ceramics (GCs), on cooling from the crystallization temperature, internal residual stresses are generated due to the difference between the thermal expansion coefficient (TEC) of the crystal phase(s) and the residual glass. These stresses could degrade or promote their mechanical properties. In this work, we varied the magnitude of the residual stresses in lithium silicate GCs by designing their microstructures. The level of internal stresses was measured using (Synchrotron) X-ray diffraction. The effects of anisotropy of thermal expansion, crystal shape, and intensity of the residual stresses were analyzed and compared using theoretical models. We extended the Hsueh-Becher model to include the thermal expansion anisotropy of the orthorhombic lithium disilicate (LS2) crystals. We found that the average residual stresses within the LS2 crystals are compressive or null (−100 to ~0) and highly anisotropic. Most importantly, within the limits of this study, we found no evidence for the influence of (compressive or null) residual stresses on the fracture toughness of the studied GCs. Within the crystal size range from 1 to 5 μm, a highly crystallized volume fraction coupled to relatively large crystals (5 μm) of high elastic modulus improved the glass-ceramic fracture toughness. This result can guide the microstructural design of novel tough GCs.     

Residual stress versus microstructural effects on the strength and toughness of phase-separated PbO–B2O3–Al2O3 glasses

A few authors have reasonably proposed that liquid–liquid phase-separated (LLPS) glasses could show improved fracture strength, S_f, and toughness, K_Ic, as the second phase could provide a barrier to crack propagation via deflection, bowing, trapping, or bridging. Due to the associated tensile or compressive residual stresses, the second phase could also act as a toughening or a weakening mechanism. In this work, we investigated five glasses of the PbO–B₂O₃–Al₂O₃ system spanning across the miscibility gap: Four of them undergo LLPS—three are binodal (two B₂O₃-rich and one PbO-rich) and one is spinodal—and one does not show LLPS (composition outside the miscibility gap). Their compositions were designed in such a way that the amorphous particles are under compressive residual stresses in some and under tensile residual stresses in others. The following mechanical properties were determined: the Vickers hardness, ball on three balls (B3B) strength, and toughness, K_Ic-SEVNB (single-edge V-notch beam [SEVNB]). The microstructures and compositions were analyzed using scanning electron microscopy with energy-dispersive X-ray spectrometry. The spinodal glass showed, by far, the best mechanical properties. Its K_Ic-SEVNB = 1.6 ± 0.1 MPa m^1/2, which embodies an increase of almost 50% over the B₂O₃-rich binodal composition, and 90% considering the PbO-rich binodal composition. Moreover, its fracture strength, S_f = 166 ± 7 MPa, is one of the highest ones ever reported for an LLPS glass. Fracture analyses evidenced that the spinodal composition exhibited the lowest net stress at the fracture point. Moreover, calculations indicate that the internal residual stress level is the lowest in the spinodal glass. The overall results indicate that the microstructural effect of the spinodal glass is the most significant factor for its superior mechanical properties. This work corroborates the idea that LLPS provides a feasible and stimulating solution to improve the mechanical properties of glasses.     

Influence of heat treatment temperature on the properties of the lithium disilicate-fluorcanasite glass-ceramics

This study aims to investigate the influence of heat treatment temperatures on the mechanical properties and chemical solubility (CS) of lithium disilicate-fluorcanasite glass-ceramics and to develop new dental materials. The glasses and glass-ceramics were prepared using CaF₂-SiO₂-CaO-K₂O-Na₂O-Li₂O-Al₂O₃-P₂O₅-based glass system using a conventional melt quenching method followed by a two-stage crystallization process. This two-stage method involves two heating temperature steps: first at a constant temperature (T_S1) of 600°C and second step at varying temperatures (T_S2) of 650, 700, 750, and 800°C. The crystallization behavior, phase formation, microstructure, translucency characteristic, density, hardness, fracture strength, and CS were investigated. It was found that the lithium disilicate crystal acted as the main crystalline phase, and the crystalline phase of fluorcanasite occurred at the heat treatment temperatures of 750 and 800°C. In addition, it was found that density, hardness, fracture strength, and CS increased while the translucency values decreased with increasing heat treatment temperatures. Furthermore, the CS increased dramatically when the fluorcanasite phases occurred in the glass-ceramic samples. The maximum density values, Vickers hardness, fracture toughness, and flexural strength are 2.56 g/cm³, 6.73 GPa, 3.38 MPa.m^1/2, and 259 MPa, respectively. These results may offer a possibility to design a new material for dental applications based on lithium disilicate-fluorcanasite glass-ceramics.     

Glass-ceramics in the CaO–MgO–Al2O3–SiO2 system as potential dental restorative materials

This paper reports on development of novel alumina-containing glass-ceramics (GCs) with a high content of Al₂O₃ (12.5 wt.%) in the CaO–MgO–Al₂O₃–SiO₂ system aimed for dental restorations. The thermal properties of the parent glasses, the microstructure and the mechanical properties of the produced sintered and crystallized GCs along with bio-inertia performance were experimentally studied. Dense, white, and bio-inert GCs, comprised of melilite, either as a single-phase or with diopside, were produced. The values of flexural strength ranged between 120 and 171 MPa, the modulus of elasticity varied between 28 and 42 GPa, while the values of the hardness and the fracture toughness (measured by the indentation–Niihara equation) ranged from 6.3 to 7.0 GPa, and from 2.6 to 2.8 MPa m^0.5, respectively. The mechanical properties of the produced GCs, after being meticulously compared with the mechanical properties of GCs of various compositions reported in literature, including commercial ones, are a good match to the properties of dental hard tissues, and satisfy the requirements of the ISO 6872 “Dentistry-Ceramic Materials”.     

Effect of substitution of ZrO2 by SnO2 on crystallization and properties of environment-friendly Li2O–Al2O3–SiO2 system (LAS) glass-ceramics

In this study, a transparent and environmentally friendly Li₂O–Al₂O₃–SiO₂ (LAS) glass-ceramic was prepared by melt-quenching and two-step heat treatment. The influence of the substitution amount of ZrO₂ by SnO₂ on the crystallization, microstructure, transparency, and mechanical properties of LAS glass and glass-ceramics was investigated by means of differential scanning calorimetry (DSC), X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Ultraviolet–visible Spectrophotometer, three-point bending strength test, and microhardness test. The results indicate that the main crystalline phase of LAS glass ceramics was a β-quartz solid solution when heat treated at 780 °C for 2 h and 870 °C for 1.5 h. When the substitution amount of ZrO₂–SnO₂ increased from 0.4 mol% to 2.5 mol%, the grain size and thermal expansion coefficient of LAS glass-ceramics first decreased and then increased, and the crystallinity first increased and then decreased. When the substitution amount of ZrO₂–SnO₂ was 0.8 mol%, the transparency of the LAS glass-ceramics was maximum, the bending strength was 96 MPa, and the Vickers hardness was 10.9 GPa.     

Preparation and characterization of alkali-free glass substrates with enhanced properties for TFT–LCDs applications

To obtain an alkali-free glass substrate with enhanced properties for thin-film transistor–liquid crystal displays (TFT–LCDs) applications, we chose a base glass composed of 3B₂O₃-15Al₂O₃-58SiO₂-22MgO-0.5SrO-1.5MgF₂ (mol%) for nucleation–crystallization. The results show that when the nucleation–crystallization processes of the base glass are 810 °C/6 h + 880 °C/6–9 h, the prepared GC/6–GC/9 glass-ceramics exhibit enhanced properties because of the precipitation of nano-sized cordierite. The transmittances in the visible range of the GC/6–GC/9 glass-ceramics exceed 85%, the densities are 2.564–2.567 g/cm³, thermal expansion coefficients are 2.934–3.059 × 10^-6/°C (25–300 °C), compressive strengths are 417–589 MPa, bending strengths are 141–259 MPa, Vickers hardnesses are 6.8–7.8 GPa, and strain points are approximately 735 °C. Considering these properties, the prepared GC/6–GC/9 glass-ceramics have good potential as candidate materials for alkali-free glass substrates. Additionally, these results demonstrate that it is feasible to improve the properties of alkali-free glass substrates by nucleation–crystallization.     

Crystallization,structure and properties of MgO-Al2O3-SiO2 highly crystalline transparent glass-ceramics nucleated by multiple nucleating agents

Generally, highly crystalline transparent glass-ceramics possess excellent physical and chemical properties compared to organic and other inorganic optical materials. We have successfully prepared highly crystalline transparent glass-ceramics in the MgO-Al₂O₃-SiO₂ system by "extreme-time" nucleation & "finite-time" crystallization processes using P₂O₅, ZrO₂ and TiO₂ as multiple nucleating agents. The results revealed that the crystallization of glass is controlled by a three-dimensional interfacial crystal growth process. These glass-ceramics mainly consisted of cordierite crystals with a residual glassy phase, and crystallinity increased with crystallization time, but light transmittance decreased with crystallization time due to enlarged grain sizes. EDS mapping revealed a uniform distribution of elements within the glass-ceramic. In the optimal preparation condition (825?°C/96?h?+?990?°C/3?h), these glass-ceramics exhibited a high crystallinity (87.3?vol. %), high transmittance (78%), and excellent mechanical properties. This work provides a roadmap for preparing highly crystalline transparent glass-ceramics for applications in optical engineering.     

Design and fabrication of Si3N4/(W,Ti)C graded nano-composite ceramic tool materials

Si₃N₄/(W, Ti)C graded nano-composite ceramic tool materials with different thickness ratios and number of layers were fabricated by hot pressing technology. The flexural strength, fracture toughness and hardness of the sintered composites were tested and the microstructure and indention cracks were observed. The experiment results showed that the five-layer graded nano-composites with a thickness ratio of 0.2, which were sintered under a pressure of 30 MPa at 1700 °C in vacuum condition for 45 min, had the optimum comprehensive mechanical properties with a flexural strength of 1080.3 MPa, a hardness of 17.64 GPa, and a fracture toughness of 10.87 MPa·m^1/2. The formation of elongated β-Si₃N₄ grains contributes to the favorable mechanical properties. The graded structure can induce residual compressive stress in the surface layer and enhance the mechanical properties. The strengthening and toughening mechanisms are a synergistic effect of intergranular and transgranular fracture, crack bridging and deflection.