The thermo-mechanical properties and ferroelastic phase transition of RENbO4 (RE = Y,La, Nd,Sm, Gd,Dy, Yb) ceramics

In this work, RENbO₄ (RE = Y, La, Nd, Sm, Gd, Dy, Yb) ceramics with low density, low Young's modulus, low thermal conductivity, and high thermal expansion have been systematically investigated, the excellent thermo-mechanical properties indicate that RENbO₄ ceramics possess the potential as the new generation of thermal barrier coatings (TBCs) materials. X-ray diffraction and Raman spectroscopy phase structure identification reveal that all dense bulk specimens obtained by high-temperature solid-state reaction belonged to the monoclinic (m) phase with C12/c1 space group. The ferroelastic domains are detected in the specimens, revealing the ferroelastic transformation between tetragonal (t) and monoclinic (m) phases of RENbO₄ ceramics. The Young's modulus and hardness of the RENbO₄ ceramics measured by the NanoBlitz 3D nanoindentation method are discussed in details, and the lower Young's modulus (60-170 GPa) and higher hardness (the maximum value reaches 11.48 GPa) indicating that higher resistance of RENbO₄ ceramics to failure and damage. Lower thermal conductivity (1.42-2.21 W [m k]⁻¹ at 500°C-900°C) and lower density (5.330-7.400 g/cm³) than other typical TBCs materials give RENbO₄ ceramics the unique advantage of being new TBCs materials. Meanwhile, the thermal expansion coefficients of RENbO₄ ceramics reach 9.8-11.6 × 10⁻⁶ k⁻¹ and are comparable or higher than other typical TBCs materials. According to the first-order derivative of the thermal expansion rate, the temperature of the ferroelastic transformation of RENbO₄ ceramics can be observed.     

Sintering,thermal expansion,and thermal transport properties of A4Ta2O9 (A= Ca,Mg) tantalates

Searching for new oxides with low thermal conductivity and high thermal expansion coefficients (TECs) as thermal barrier coatings (TBCs) is vital for the development of highly efficient gas turbines and aeroengines. We report the densification sintering, high TECs, and low thermal conductivity of A₄Ta₂O₉ (A = Ca, Mg) tantalates. The best sintering temperature of dense A₄Ta₂O₉ ceramics was determined via an optical contact angle tester, and samples with a relative density of 99.8% were synthesized via spark plasma sintering (SPS). The hardness (9–10 GPa), Young's modulus (172.7–211.8 GPa) and fracture toughness (1.5–1.6 MPa m^1/2) of the A₄Ta₂O₉ ceramics are primarily affected by the bonding strength. Furthermore, we studied the thermal transport properties of A₄Ta₂O₉. The low thermal conductivity (1.78–1.93 W m^?1 K^?1 at 900 °C), extraordinary phase stability, and high TECs (11.4–11.8 × 10^?6 K^?1 at 1200 °C) of A₄Ta₂O₉ ceramics make them candidate TBCs with high operating temperatures.     

Mechanical properties,thermal expansion performance and intrinsic lattice thermal conductivity of AlMO4 (M=Ta,Nb) ceramics for high-temperature applications

The vital thermo-mechanical properties of thermal and environment barrier coatings (TBCs/EBCs) include high hardness, low Young's modulus, matching thermal expansion coefficients (TECs) with substrate and low thermal conductivity. The effect of distortion degree of crystal structure on thermo-mechanical properties of AlMO₄ (M=Ta, Nb) ceramics are assessed in this work. AlMO₄ ceramics display modest TECs and no phase transformation is detected from room temperature to 1200?℃. The experiment thermal conductivity can be dropped further as the theoretical minimum thermal conductivity of AlTaO₄ and AlNbO₄ is 1.48?W?m^?1 K^?1 and 1.05?W?m^?1 K^?1, respectively. The temperature dependent phonon thermal diffusivity of AlMO₄ ceramics has been confirmed; the intrinsic lattice thermal conductivity is determined. The extraordinary thermo-mechanical properties make it clear that AlMO₄ ceramics are suitable for high-temperature applications.     

First-principles study of thermophysical properties of polymorphous YTaO4 ceramics

Yttrium tantalate ceramics with ferroelasticity are potential candidates for thermal barrier coating (TBC) ceramics. During the phase transition process, there are three main phases with monoclinic (I2/a), monoclinic-prime (P2/a), and tetragonal structures (I₄₁/a), and a comprehensive understanding of their thermophysical properties is required. In this study, the thermal and mechanical properties of polymorphous yttrium tantalate (YTaO₄) ceramics are systematically investigated under finite temperature by performing first-principles calculations combined with quasi-harmonic approximation. The first-principle study results show that the volume change from M' to T phase is 12.85 Å³ to 12.95 Å³ per atom, whereas the T to M is 12.95 Å³ to 12.84 Å³ per atom, and the change is less than 1%, showing that this process produces almost no volume change. However, the thermal expansion coefficients (TECs) and Young's modulus vary greatly, the TECs value of M YTaO₄ is about 11.13 × 10⁻⁶ K⁻¹, which is smaller than T YTaO₄ as the value 12.01 × 10⁻⁶ K⁻¹, and the Young's modulus values of M, M', and T phases are 140.34, 156.68, and 123.29 GPa, respectively. Lastly, the calculated O–Ta bond is stronger than the O–O and O–Y bonds according to the mean bond population and average bond length, resulting in a higher modulus. This work will not only expand the internal mechanism of the thermophysical properties of YTaO₄, but also provides support for the design and application of TBC systems.     

Synergistic modification of properties in Ba[(Zn0.8Mg0.2)1/3Nb2/3]O3 ceramics through ordered domain engineering

The ordered domain engineering was investigated for Ba[(Zn_0.8Mg_0.2)_1/3Nb_2/3]O₃ microwave dielectric ceramics to synergistically modify the physical properties especially the temperature coefficient of resonant frequency τ_f and quality factor Q value together with the thermal conductivity. The ordered domain structure could be tailored and controlled by the post-densification annealing, and the fine ordered domain structures with high ordering degree and low-energy domain boundary were obtained in the present ceramics annealed around 1400°C for 24 h, where the Qf value was improved from 51 000 to 118 000 GHz, τ_f was suppressed from 30 to 25.5 ppm/°C. Moreover, the thermal conductivity at room temperature was increased from 3.79 to 4.30 W m⁻¹ K⁻¹, and the Young's modulus was improved from 98 to 214 GPa. The present work provided a promising approach for synergistic modification of physical properties in Ba-based complex perovskite microwave dielectric ceramics.     

High-entropy ferroelastic rare-earth tantalite ceramic: (Y0.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4

In this study, high-entropy rare-earth tantalate ceramics (Y_0.2Ce_0.2Sm_0.2Gd_0.2Dy_0.2)TaO₄ ((5RE_0.2)TaO₄) have been successfully fabricated. The possibility of formation of (5RE_0.2)TaO₄ was verified via first-principles calculations. In addition, the phase structure, ferroelastic toughening mechanism, thermophysical, and mechanical properties were systematically investigated. The (5RE_0.2)TaO₄ ceramics have lower phonon thermal conductivity (1.2–2.6 W·m^–1·K^–1) in the entire temperature range than that of RETaO₄ and YSZ. (5RE_0.2)TaO₄ has a higher fracture toughness and lower brittleness index than YSZ. The thermal expansion coefficients of (5RE_0.2)TaO₄ are as high as 10.3 × 10^-6 K^–1 at 1200°C and Young's modulus is 66–189 GPa, and thus, (5RE_0.2)TaO₄ possesses great potential for application in thermal barrier coatings (TBCs).     

Magneto-optical,thermal, and mechanical properties of polycrystalline Tb3Al5O12 transparent ceramics

Terbium aluminum garnet (Tb₃Al₅O₁₂, TAG) ceramics have become a promising magneto-optical material owing to the outstanding comprehensive performance, including the magneto-optical, thermal, and mechanical properties. Fine-grained TAG ceramics with high optical quality and mechanical properties have attracted much attention. In this study, TAG ceramics with fine grains and high optical quality are fabricated successfully by a two-step sintering method from co-precipitated nano-powders. After pre-sintered at 1525°C in vacuum and hot isostatic pressed at 1600°C, the in-line transmittance of TAG ceramics reaches 81.8% at 1064 nm, and the average grain size is 7.1 μm. The Verdet constant of TAG ceramics is −179.6 ± 4.8 rad T⁻¹ m⁻¹ at 633 nm and −52.1 ± 1.9 rad T⁻¹ m⁻¹ at 1064 nm, higher than that of commercial Tb₃Ga₅O₁₂ crystals. The thermal conductivity of TAG ceramics is determined from 25 to 450°C, and the result is 5.12 W m⁻¹ K⁻¹ at 25°C and 3.61 W m⁻¹ K⁻¹ at 450°C. A comparison of mechanical properties between large- and fine-grained TAG ceramics fabricated under different conditions is conducted. The fine-grained TAG ceramics possess a bending strength of 226.3 ± 16.4 MPa, which is 9.7% higher than that of the large-grained ceramics. These results indicate that reducing the grain size on the premise of high optical quality helps improve the comprehensive performance of TAG ceramics.     

Spark plasma sintering of (5RE.2)Ta3O9 high-entropy ceramics and their thermal properties

Six rare-earth tantalate high-entropy ceramics of (5RE_.2)Ta₃O₉ (RE represents any five elements selected from La, Ce, Nd, Sm, Eu, Gd) were designed and prepared by spark plasma sintering process at 1400°C in this study. The (5RE_.2)Ta₃O₉ ceramics only consist of a single-phase solid solution with perovskite structure. Their relative densities are all above 90%, and the average grain size is in the range of 1.47–2.92 μm. The thermal conductivity of (5RE_.2)Ta₃O₉ ceramics is in 2.24–1.90 W m⁻¹ K⁻¹ (25°C–500°C), which is much lower than that of yttria-stabilized zirconia. In six samples, (La_.2Nd_.2Sm_.2Gd_.2Eu_.2)Ta₃O₉ possesses a thermal conductivity of 1.90 W m⁻¹ K⁻¹, a thermal expansion coefficient of 3.47 × 10⁻⁶ K⁻¹ (500°C), a Vickers hardness of about 7.33 GPa, and a fracture toughness of about 5.20 MPa m^1/2, which are suitable for its application as thermal barrier coatings.     

New class of high-entropy rare-earth niobates with high thermal expansion and oxygen insulation

Tailoring the structure and properties of materials using the high-entropy (HE) effect is of significant interest in the fields of environmental and thermal barrier coatings (TBCs). In this work, a new class of dense HE rare-earth niobates was successfully prepared by a solid-phase reaction method, including (Sm_1/5Dy_1/5Ho_1/5Er_1/5Yb_1/5)NbO₄ (5HERN), (Sm_1/6Dy_1/6Ho_1/6Er_1/6Yb_1/6Lu_1/6)NbO₄ (6HERN), (Sm_1/7Dy_1/7Ho_1/7Er_1/7Yb_1/7Lu_1/7Gd_1/7)NbO₄ (7HERN), and (Sm_1/8Dy_1/8Ho_1/8Er_1/8Yb_1/8Lu_1/8Gd_1/8Tm_1/8)NbO₄ (8HERN), along with eight single rare-earth niobates (RENbO₄, RE = Sm, Dy, Ho, Er, Yb, Lu, Gd, and Tm). X-ray diffraction analysis showed that 5–8HERN are single-phase solid solutions with a monoclinic structure (space group C12/c1). The thermal expansion coefficients of 7HERN and 8HERN exceed 11 × 10⁻⁶ K⁻¹ at 1200°C and are much higher than those of the RENbO₄ compositions (10.13–10.74 × 10⁻⁶ K⁻¹) and other some HE rare-earth oxides (10.27–10.87 × 10⁻⁶ K⁻¹). Importantly, 5–8HERN have lower oxygen-ion conductivity and higher activation energy than yttrium-stabilized zirconia (YSZ) and the RENbO₄ compositions. The oxygen-ion conductivity of 5HERN (7.52 × 10⁻⁷ S cm⁻¹, 900°C) was 10⁵ times lower than that of YSZ (0.01 S cm⁻¹, 750°C). The hardness of 5–8HERN is ∼7.81–8.46 GPa and these compositions have low intrinsic lattice thermal conductivity at high temperature (1.28–1.69 W m⁻¹ K⁻¹ at 900°C). The mechanism by which the HE effect improved the material properties was elucidated. Young's modulus, hardness, thermal expansion coefficient, and intrinsic lattice thermal conductivity are linearly related to the mass, size, and distortion degree of samples. In contrast, the oxygen-ion conductivity depends on both the degrees of disorder and distortion and the oxygen-ion vacancy concentration. Based on their overall performance, especially their high thermal expansion coefficients and excellent oxygen-barrier performance, HE rare-earth niobates show potential for further development as TBC materials.     

Preparation of ultralow thermal conductivity (Mg0.5Ca0.3Ba0.2) (AlSi)2O8 ceramics

A type of nonequimolar multicomponent ceramic solid solution (Mg_0.5Ca_0.3Ba_0.2) (AlSi)₂O₈ with a low thermal conductivity was prepared through solid-state synthesis. Results show that the (Mg_0.5Ca_0.3Ba_0.2) (AlSi)₂O₈ solid solution exhibits excellent high-temperature stability and an ultralow thermal conductivity (.3676 W m⁻¹ K⁻¹), far lower than widely used 3YSZ (2.9 W m⁻¹ K⁻¹), La₃NbO₇ (1.5 W m⁻¹ K⁻¹), and Gd₂Zr₂O₇ (1.28 W m⁻¹ K⁻¹). Furthermore, the Young modulus of the final product is 64.56 GPa. Therefore, the proposed ceramic solid solution provides a new research direction for ultralow thermal conductivity materials and has a practical application value for the field of wall thermal insulation.     

A new type of Sr(Zr0.2Hf0.2Ce0.2Yb0.2Me0.2)O3−x (Me = Y,Gd) high-entropy ceramics used in thermal barrier coatings

Seeking for new ceramics with excellent thermophysical properties as thermal barrier coatings candidate materials has become a hot research field. In this study, Sr(Zr_0.2Hf_0.2Ce_0.2Yb_0.2Me_0.2)O_3−x high-entropy ceramic powders were successfully synthesized by the method of solid-state reaction, and the ceramics with single phase were prepared by pressureless sintering at 1600°C. The phase composition, microstructure, element distribution, high-temperature thermal stability, and thermophysical properties of the ceramics were studied. The results showed that Sr(Zr_0.2Hf_0.2Ce_0.2Yb_0.2Me_0.2)O_3−x ceramics were composed of SrZrO₃ phase and the second phase of AB₂O₄ spinel (i.e., SrY₂O₄ and SrGd₂O₄). The content of the second phase was gradually increased after heat treatment at 1400°C, which significantly improved the thermophysical and mechanical properties of the ceramics. The microhardness and fracture toughness of the ceramics were improved compared with that of SrZrO₃. The thermal conductivities of Sr(Zr_0.2Hf_0.2Ce_0.2Yb_0.2Me_0.2)O_3−x (Me = Y, Gd) ceramics were 1.30 and 1.28 W m⁻¹ K⁻¹ at 1000°C, which were about 35% and 40% lower than that of SrZrO₃ (1.96 W m⁻¹ K⁻¹) and yttria-stabilized zirconia (2.12 W m⁻¹ K⁻¹), respectively. The thermal expansion coefficients of Sr(Zr_0.2Hf_0.2Ce_0.2Yb_0.2Me_0.2)O_3−x (Me = Y, Gd) ceramics were 12.8 × 10⁻⁶ and 14.1 × 10⁻⁶ K⁻¹ at 1300°C, respectively, which was more closer to the superalloys compared with SrZrO₃ ceramic (11.0 × 10⁻⁶ K⁻¹).     

Fiber Reinforced Polyimide Aerogel Composites with High Mechanical Strength for High Temperature Insulation

Glass fiber/polyimide aerogel composites are prepared by adding glass fiber mat to a polyimide sol derived from diamine, 4,4′‐oxydianiline, p‐phenylene diamine, and dianhydride, 3,3′,4,4′‐biphenyltetracarboxylic dianhydride. The fiber felt acts as a skeleton for support and shaping, reduces aerogel shrinkage during the preparation process, and improves the mechanical strength and thermal stability of the composite materials. These composites possess a mesoporous structure with densities as low as 0.143–0.177 g cm^?3, with the glass fiber functioning to improve the overall mechanical properties of the polyimide aerogel, which results in its Young's modulus increasing from 42.7 to 113.5 MPa. These composites are found to retain their structure after heating at 500 °C, in contrast to pure aerogels which decompose into shrunken ball‐like structures. These composites maintain their thermal stability in air and N₂ atmospheres, exhibiting a low thermal conductivity range of 0.023 to 0.029 W m^?1 K^?1 at room temperature and 0.057to 0.082 W m^?1 K^?1 at 500 °C. The high mechanical strengths, excellent thermal stabilities, and low thermal conductivities of these aerogel composites should ensure that they are potentially useful materials for insulation applications at high temperature.     

Thermal stability and thermal conductivity of stacked Cs intercalated layered niobate

Layered materials exhibit competitively low thermal conductivity along the out-of-plane direction. The solution process is a promising method for preparing stacked structures. However, the thermal stability of the layered materials is poor after processing in solution, thus hindering their applications at high temperatures. One of the solutions to improve the thermal stability of layered structures is to expand the interlayer distance by inserting large-size metal ions. In this work, we studied the thermal properties of Cs⁺ intercalated layered niobate obtained by the ion-exchanged process. The layered structure of the Cs⁺ intercalated layered niobate survives after thermal treatment even at 1200 °C. The room temperature thermal conductivity of as prepared stacked Cs–HCa₂Nb₃O₁₀ is as low as 0.11 W m⁻¹ k⁻¹. Upon thermal annealing, the thermal conductivity increases. After annealing at 1200 °C, the value is 0.90 W m⁻¹ k⁻¹. The finding suggests Cs⁺ intercalated layered niobate is a promising material for high-temperature insulation applications.     

Impact of ZrO2 alloying on thermo-mechanical properties of Gd3NbO7

The ZrO₂ alloying effect is widely used to optimize the thermo-mechanical properties of potential thermal barrier coatings. In this study, dense x mol% ZrO₂-Gd₃NbO₇ with C222₁ space group were manufactured via a solid-state reaction. The crystalline structure was determined through X-ray diffraction and Raman spectroscopy, when the surface morphology was observed by scanning electron microscopy. ZrO₂-Gd₃NbO₇ had identical orthorhombic crystal structures, and there was no second phase. The crystalline structure of ZrO₂-Gd₃NbO₇ shrunk with the increasing ZrO₂ content as indicated by XRD and Raman results. The heat capacity and thermal diffusivity of ZrO₂-Gd₃NbO₇ were 0.31–0.43 J g⁻¹ K⁻¹ (25–900 °C) and 0.25–0.70 mm²/s (25–900 °C), respectively. It was found that ZrO₂-Gd₃NbO₇ had much lower thermal conductivity (1.21–1.82 W m⁻¹ K⁻¹, 25–900 °C) than YSZ (2.50–3.00 W m⁻¹ K⁻¹) and La₂Zr₂O₇ (1.50–2.00 W m⁻¹ K⁻¹). The thermal expansion coefficients (TECs) were higher than 10.60 × 10⁻⁶ K⁻¹ (1200 °C), which were better than that of YSZ (10.00 × 10⁻⁶ K⁻¹) and La₂Zr₂O₇ (9.00 × 10⁻⁶ K⁻¹). The mechanical properties of Gd₃NbO₇ change little with the increasing ZrO₂ content, Vickers hardness was about 10 GPa, and Young's modulus was about 190 GPa, which was lower than YSZ (240 GPa). Compared with previous work about alloying effects, much lower thermal conductivity was obtained. Due to the high melting point, high hardness, low Young's modulus, ultralow thermal conductivity and high TECs, it is believed that ZrO₂-Gd₃NbO₇ is promising TBCs candidate.     

Solvothermal-derived multicomponent rare-earth cerate ceramics toward remarkable thermophysical properties

The multicomponent rare-earth cerate (Y_0.2La_0.2Nd_0.2Sm_0.2Eu_0.2)₂Ce₂O₇ (5RE₂Ce₂O₇) ceramics were successfully fabricated through solvothermal method and the following calcination process. The microstructure and phase composition of the as-obtained products were systematically characterized via SEM, TEM and XRD techniques. The results showed that the as-synthesised 5RE₂Ce₂O₇ has a single-phase fluorite-type crystal structure with the particle size of approximately 200 nm. Furthermore, the as-synthesised 5RE₂Ce₂O₇ demonstrated lower thermal conductivity (1.9–1.26 W m^?1·K^?1 at 25–1000 °C), higher thermal expansion coefficients (CTEs, 12.48 × 10^?6 K^?1 at 1000 °C), and outstanding mechanical properties including large Young's modulus (248.0 ± 0.35 GPa) and high fracture toughness (2.4 ± 0.21 MPam^1/2). The excellent properties of the as-synthesised 5RE₂Ce₂O₇ demonstrates its potential application as a new type of next-generation TBCs.     

Multiphonon scattering mechanisms to limit thermal conductivity in weberite RE3NbO7: A case study of (La1-xGdx)3NbO7 ceramics

The management of thermal conductivity is of significant scientific interest, particularly for thermal barrier coatings (TBCs). Multifarious strategies have been used to regulate heat transportation, but it is hard to achieve limit thermal conductivity at elevated temperatures. A systematical investigation of weberite (La_1-xGd_x)₃NbO₇ was thus performed, and multiphonon scattering mechanisms were introduced to achieve limit thermal conductivity (0.92 W m^?1 K^?1). Phonon point defect scattering process accounted for thermal conductivity reduction at low temperatures. Additionally, lattice softening strongly contributed to the reduction of high-temperature thermal conductivity, and solid and stiff chemical bonds were beneficial for inhibiting thermal radiative conductivity. A novel strategy was presented to modify thermal transportation property of weberite RE₃NbO₇ ceramics. Also, the hardness, toughness, and modulus were improved to promote engineering applications of weberite RE₃NbO₇. This study also illuminates novel paths for thermal management and mechanical properties manipulation of TBCs, thermoelectric materials, and microelectronics.     

Fabrication of Si3N4 ceramics substrates with high thermal conductivity by tape casting and gas pressure sintering

In this paper, high thermal conductivity Si₃N₄ ceramics were successfully fabricated through exploring and optimizing the tape casting process. The impact of various organic additives on the rheological characteristics of Si₃N₄ slurry was explored, and the pore size distribution and microstructure of the green tapes at different solid loadings were investigated, as well as the microstructure of Si₃N₄ ceramics. Green tapes with a narrow pore size distribution, a small average pore size, and a high density of 1.88 g cm⁻³ were prepared by the investigation and optimization of the Si₃N₄ slurry formulation. After gas pressure sintering, Si₃N₄ ceramics with a density of 3.23 g cm⁻³, dimensions of 78 mm × 78 mm, and a thickness of 0.55 mm were obtained. The microstructure of the Si₃N₄ ceramics showed a bimodal distribution and a low content of glassy phases. The thermal conductivity of the Si₃N₄ ceramics was 100.5 W m⁻¹ K⁻¹, the flexural strength was 735 ± 24 MPa, and the fracture toughness was 7.17 MPa m^1/2.     

High-entropy (Ho0.2Y0.2Dy0.2Gd0.2Eu0.2)2Ti2O7/TiO2 composites with excellent mechanical and thermal properties

High-performance ceramics with low thermal conductivity, high mechanical properties, and idea thermal expansion coefficients have important applications in fields such as turbine blades and automotive engines. Currently, the thermal conductivity of ceramics has been significantly reduced by local doping/substitution or further high-entropy reconfiguration of the composition, but the mechanical properties, especially the fracture toughness, are insufficient and still need to be improved. In this work, based on the high-entropy titanate pyrochlore, TiO₂ was introduced for composite toughening and the high-entropy (Ho_0.2Y_0.2Dy_0.2Gd_0.2Eu_0.2)₂Ti₂O₇-xTiO₂ (x = 0, 0.2, 0.4, 1.0 and 2.0) composites with high hardness (16.17 GPa), Young's modulus (289.3 GPa) and fracture toughness (3.612 MPa·m^0.5), low thermal conductivity (1.22 W·m⁻¹·K⁻¹), and thermal expansion coefficients close to the substrate material (9.5 ×10⁻⁶/K) were successfully prepared by the solidification method. The fracture toughness of the composite toughened sample is 2.25 times higher than that before toughening, which exceeds most of the current low-thermal conductivity ceramics.     

Moisture-Resistant and Mechanically Strong Polyimide-Polymethylsilsesquioxane Hybrid Aerogels with Tunable Microstructure

Moisture-resistant and mechanically strong polyimide (PI)-polymethylsilsesquioxane hybrid aerogels with doubly cross-linked structures are synthesized through sol–gel technology and supercritical CO₂ fluid drying. By using bis(trimethoxysilylpropyl) amine as a cross-linker, the end-capped polyamide acid derived from biphenyl-3,3′,4,4′-tetracarboxylic dianhydride and 4,4′-oxydianiline is cross-linked with a silica network using methyltrimethoxysilane as the silica source precursor. The resultant hybrid aerogels show low density (0.12–0.15 g cm⁻³), low thermal conductivity (0.032–0.049 W m⁻¹ K⁻¹), high hydrophobicity (125–140°) and good thermal stability (above 435 °C) with tunable microstructure. With the increase of silica sol volume, the microstructure of hybrid aerogels transforms from fibrous network to hierarchical microstructure. Aerogels with high content of silica sol exhibit good moisture resistance, high Young's modulus (Max. 19.6 MPa), and high specific modulus (Max. 131 kN m kg⁻¹), which are attributed to their unique hierarchical microstructure with a sheet skeleton. These hybrid aerogels are promising in the fields of thermal insulation, aerospace applications and so on.