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1.
《Ceramics International》2023,49(12):20406-20418
Herein, we present the structural evolution of polymer-derived SiOC ceramics with the pyrolysis temperature and the corresponding change in their microwave dielectric properties. The structure of the SiOC ceramics pyrolyzed at a temperature lower than 1200 °C is amorphous, and the corresponding microwave complex permittivity is pretty low; thus, the ceramics exhibit wave transmission properties. The Structural arrangement of free carbon in the SiOC ceramics mainly happens in the temperature range of 1200 °C-1300 °C due to the separation from the Si–O–C network and graphitization, while the structural arrangement of the Si-based matrix mainly occurs in the range of 1300 °C-1400 °C owing to the separation of SiC4 from the Si–O–C network to form nanocrystalline SiC. In pyrolysis temperature range of 1200 °C-1400 °C, the microwave permittivity of SiOC shows negligible change. At a pyrolysis temperature exceeding 1400 °C, the carbothermal reaction of free carbon and the Si–O backbone becomes significant, leading to the formation of crystalline SiC. The as-formed SiC and residual defective carbon improve the polarization loss of SiOC ceramics. In this case, the SiOC ceramics show significantly increased complex permittivity, exhibiting electromagnetic absorption characteristics. These characteristics promote the application of polymer-derived SiOC ceramics to high-temperature electromagnetic absorption materials.  相似文献   

2.
《Ceramics International》2020,46(8):12172-12179
In this work, diphasic mullite (3Al2O3·2SiO2) nanofibers with good homogeneity were prepared by electrospinning method. Aluminum nitrate (AN) and aluminum isopropoxide (AIP) were used as alumina sources, commercial colloidal silica as silica source, and polyvinyl alcohol (PVA) as polymer additive. Precursor nanofibers with continuous and uniform structures were acquired at mass ratio of PVA to precursor sol from 0.06 to 0.09. γ-Al2O3 phase was obtained at 878 °C and mullite phase formed at 1322 °C upon heating of the precursor under air atmosphere. Calcined samples suggested mullite as dominant phase at 1300 °C and amorphous SiO2 could even exist at 1400 °C. As-prepared nanofibers possessed continuous structures with subequal average diameters at 900–1200 °C. However, such morphological characteristics were lost at temperatures above 1300 °C due to rapid growth of crystal grains. Al and Si elements were uniformly distributed in fibers and mixed at nanoscale, confirming homogeneity and diphasic features of nanofibers.  相似文献   

3.
The mullite and ytterbium disilicate (β-Yb2Si2O7) powders as starting materials for the Yb2Si2O7/mullite/SiC tri-layer coating are synthesized by a sol–gel method. The effect of SiC whiskers on the anti-oxidation properties of Yb2Si2O7/mullite/SiC tri-layer coating for C/SiC composites in the air environment is deeply studied. Results show that the formation temperature and complete transition temperature of mullite were 800–1000 and 1300°C, respectively. Yb2SiO5, α-Yb2Si2O7, and β-Yb2Si2O7 were gradually formed between 800 and 1000°C, and Yb2SiO5 and α-Yb2Si2O7 were completely transformed into β-Yb2Si2O7 at a temperature above 1200°C. The weight loss of Yb2Si2O7/(SiCw–mullite)/SiC tri-layer coating coated specimens was 0.15 × 10−3 g cm−2 after 200 h oxidation at 1400°C, which is lower than that of Yb2Si2O7/mullite/SiC tri-layer coating (2.84 × 10−3 g cm−2). The SiC whiskers in mullite middle coating can not only alleviate the coefficient of thermal expansion difference between mullite middle coating and β-Yb2Si2O7 outer coating, but also improve the self-healing performance of the mullite middle coating owing to the self-healing aluminosilicate glass phase formed by the reaction between SiO2 (oxidation of SiC whiskers) and mullite particles.  相似文献   

4.
Nitrogen (N)-doped conductive silicon carbide (SiC) of various electrical resistivity grades can satisfy diverse requirements in engineering applications. To understand the mechanisms that determine the electrical resistivity of N-doped conductive SiC ceramics during the fast spark plasma sintering (SPS) process, SiC ceramics were synthesized using SPS in an N2 atmosphere with SiC powder and traditional Al2O3–Y2O3 additive as raw materials at a sintering temperature of 1850–2000°C for 1–10 min. The electrical resistivity was successfully varied over a wide range of 10−3–101 Ω cm by modifying the sintering conditions. The SPS-SiC ceramics consisted of mainly Y–Al–Si–O–C–N glass phase and N-doped SiC. The Y–Al–Si–O–C–N glass phase decomposed to an Si-rich phase and N-doped YxSiyCz at 2000°C. The Vickers hardness, elastic modulus, and fracture toughness of the SPS-SiC ceramics varied within the ranges of 14.35–25.12 GPa, 310.97–400.12 GPa, and 2.46–5.39 MPa m1/2, respectively. The electrical resistivity of the obtained SPS-SiC ceramics was primarily determined by their carrier mobility.  相似文献   

5.
To obtain composite ceramics with excellent thermal shock resistance and satisfactory high?temperature service performance for solar thermal transmission pipelines, SiC additive was incorporated into Al2O3?mullite?ZrO2 composite ceramics through a pressureless sintering process. The effect of the SiC additive on thermal shock resistance was studied. Also, the variations in the microstructure and physical properties during thermal cycles at 1300 °C were discussed. The results showed that both thermal shock resistance and thermal cycling performance could be improved by adding 20 wt% SiC. In particular, the sample with 50 wt% Al2O3, 35 wt% Coal Series Kaolin (CSK), 15 wt% partially yttria?stabilized zirconia (PSZ), and 20 wt% SiC additional (denoted as sample A2) exhibited the best overall performance after firing at 1600 °C. Furthermore, the bending strength of sample A2 increased to 124.58 MPa, with an increasing rate of 13.63% after 30 thermal shock cycles. The increase in thermal conductivity and the formation of mullite were the factors behind the enhancement of thermal shock resistance. During the thermal cycles, the oxidation of SiC particles was favorable as it increased the microstructure densification and also facilitated the generation of mullite, which endowed the composite ceramics with a self?reinforcing performance.  相似文献   

6.
《Ceramics International》2017,43(4):3741-3747
Silicon carbide reticulated porous ceramics (SiC RPCs) with three-layered struts were fabricated by polymer replica method, followed by infiltrating alumina slurries containing silicon (slurry-Si) and andalusite (slurry-An), respectively. The effects of composition of infiltration slurries on the strut structure, mechanical properties and thermal shock resistance of SiC RPCs were investigated. The results showed that the SiC RPCs infiltrated with slurry-Si and slurry-An exhibited better mechanical properties and thermal shock resistance in comparison with those of alumina slurry infiltration, even obtained the considerable strength at 1300 °C. In slurry-Si, silicon was oxidized into SiO2 in the temperature range from 1300 °C to 1400 °C and it reacted with Al2O3 into mullite phase at 1450 °C. Meantime, the addition of silicon in slurry-Si could reduce SiC oxidation of SiC RPCs during firing process in contrast with alumina slurry. With regard to slurry-An, andalusite started to transform into mullite phase at 1300 °C and the secondary mullitization occurred at 1450 °C. The enhanced mechanical properties and thermal shock resistance of SiC RPCs infiltrated alumina slurries containing silicon and andalusite were attributed to the optimized microstructure and the triangular zone (inner layer of strut) with mullite bonded corundum via reaction sintering. In addition, the generation of residual compressive stress together with better interlocked needle-like mullite led to the crack-deflection in SiC skeleton, thus improving the thermal shock resistance of obtained SiC RPCs.  相似文献   

7.
The Si/B/C/N/H polymer T2(1), [B(C2H4Si(CH3)NH)3]n, was reacted with different amounts of H3Al·NMe3 to produce three organometallic precursors for Si/B/C/N/Al ceramics. These precursors were transformed into ceramic materials by thermolysis at 1400 °C. The ceramic yield varied from 63% for the Al-poor polymer (3.6 wt.% Al) to 71% for the Al-rich precursor (9.2 wt.% Al). The as-thermolysed ceramics contained nano-sized SiC crystals. Heat treatment at 1800 °C led to the formation of a microstructure composed of crystalline SiC, Si3N4, AlN(+SiC) and a BNCx phase. At 2000 °C, nitrogen-containing phases (partly) decomposed in a nitrogen or argon atmosphere. The high temperature stability was not clearly related to the aluminium concentration within the samples. The oxidation behaviour was analysed at 1100, 1300, and 1500 °C. The addition of aluminium significantly improved the oxide scale quality with respect to adhesion, cracking and bubble formation compared to Al-free Si(/B)/C/N ceramics. Scale growth rates on Si/B/C/N/Al ceramics at 1500 °C were comparable with CVD–SiC and CVD–Si3N4, which makes these materials promising candidates for high-temperature applications in oxidizing environments.  相似文献   

8.
Silicon-containing ceramics fibers are ideal candidates for thermal resistance due to their incomparable thermo-stability and chemical stability. Research into anti-oxidation behavior of silicon-containing ceramics through metal elements doping is important for the application in extreme high-temperature environment. Thus, uniform belts-like Zr-doped SiOC ceramics fibers were successfully prepared by electrospinning and polymer-derived ceramics routine with polycarbosilane (PCS) and zirconium butoxide as precursors. The morphology and dimension of the fibers were conveniently controlled by tuning PCS concentration, types of spinning additives and pyrolysis temperature. The ceramics fibers were composed of SiC, ZrO2 and SiO2 crystals, accompanied with amorphous SimZrnCxOy. The structure and compositions realized the excellent thermal stability above 1300°C and the enhanced flexibility. The obtained fibers maintained ultra-low thermal conductivity of .038–.053 W/(m·K). Thus, the materials were anticipated to be ideal for the thermal insulation up to 1400°C or higher.  相似文献   

9.
《Ceramics International》2023,49(3):4082-4090
Hollow silicon oxycarbide (SiOC) ceramic microspheres were synthesized through solvothermal process of vinyltriethoxysilane in NaOH solution with subsequent pyrolysis at high temperature. Increasing the synthesis temperature not only reduces the Si–C bond and C content in SiOC ceramics, but also transforms the amorphous SiOC ceramics into cristobalite SiO2 after carbonization. The rearrangement reaction of oxygen-enriched structural units results in the increase of SiO2C2 unit. No phase separation occurs at 1400 °C, and SiC nanocrystals are mainly come from the carbothermal reduction reaction of SiO2 with free C. The size change of SiO2 nanograins were further investigated by HF etching. The porous carbon is obtained after removal of SiO2, while HF etching has no effect on the structure of free C. The C content affects the structure evolution of SiOC ceramics significantly. Although the size of SiO2 grows as increase of pyrolysis temperature, the high C content inhibits the crystallization and growth of SiO2 during the pyrolysis process.  相似文献   

10.
Barium strontium alumino silicate (BSAS); (Ba0.6Sr0.4Al2Si2O8) was synthesized through solid state reaction between BaCO3, SrCO3, Al2O3 and SiO2 subjected to wet milling in isopropanol for about 24 h. The sequence of the solid state reaction was studied by subjecting to DG/DTG from room temperature to 1550 °C. The crystallographic phase evolution was confirmed by X-ray diffraction of the powders calcined in the range 1000 to 1300 °C for 2 h. The monoclinic celsian phase obtained at 1300 °C, pelletized through uniaxial pressing was sinterable to 67 to 78% density in the temperature range of 1300 to 1500 °C. The density improved to 75 to 94% after ball milling for 76 h, while ZrO2 addition further improved the density by 2%. The celcian phase of BSAS was dispersed in isopropyl alcohol, milled for about 24 h and spray coated on to plain SiC and mullite precoated SiC substrates. Sintering of coated samples and characterization for weight gain/loss, microstructure, scratch test prove that mullite + BSAS coating is more effective than single layer coating of BSAS on SiC substrates.  相似文献   

11.
《Ceramics International》2023,49(13):22022-22029
The in-situ controllable synthesis of AlN–SiC solid solution reinforcement in large-sized Al–Si3N4–Al2O3 composite refractory by two-steps nitriding sintering was examined. In the first step, a dynamic Al@AlN structure was constructed in the composite by pre-nitriding at 580 °C. During the subsequent sintering process, it cracked above ∼900 °C, and micronized Al cluster (mixture of droplets and vapor) was extracted out gradually. As a result, multiple AlN mesophases were formed through different reaction paths, including i) initial AlN shell formed by solid Al with N2, ii) reaction of Al cluster with N2, and iii) reaction of Al cluster with Si3N4 from 900 °C to 1500 °C. The Si3N4 precursor serves as both a solid nitrogen source and an active Si source, and the controllable reaction between Al and Si3N4 leading to uniformly distributed AlN and Si mesophases. AlN–SiC solid solution is significantly formed when liquid Si appears. The shell, granule and whisker SiC–AlN solid solution were observed mainly depending on the dynamic AlN mesophase. The SiC–AlN solid solution reinforced Al2O3 materials is a novel promising refractory for large-scale blast furnace lining.  相似文献   

12.
In this research, for studying the influence of size and heat treatment temperature of initial Al(OH)3 on the physical properties of porous mullite ceramics, porous mullite ceramics were prepared by in situ reaction sintering of amorphous silica and treated Al(OH)3. The transition phases χ-Al2O3, к-Al2O3, and stable phase α-Al2O3 can be obtained in turn when the treatment temperature of raw Al(OH)3 is 500, 1000, and 1500°C, respectively. The coarser the raw Al(OH)3, the higher the strength of porous mullite ceramics. When the sintering temperature is 1500°C, the bending strengths of PS500-C, PS1000-C, and PS1500-C (PSx-C represents that the specimen was prepared by the coarse grade Al(OH)3, which was previously treated at x°C) are 40.3 ± 2.1, 54.9 ± 5.2, and 64.8 ± 4.8 MPa, respectively. In addition, although the activated Al2O3 can decrease the formation temperature (∼100°C) of porous mullite ceramics, the strength and density of porous mullite ceramics prepared by activated Al2O3 will decrease at the same sintering temperature. It is believed that the increase of defects and pores during the phase transformation should be responsible for this phenomenon.  相似文献   

13.
We present here the single-source-precursor synthesis of Fe3Si and Fe5Si3-containing SiOC ceramic nanocomposites and investigation of their magnetic properties. The materials were prepared upon chemical modification of a hydroxy- and ethoxy-substituted polymethylsilsesquioxane with iron (III) acetylacetonate (Fe(acac)3) in different amounts (5, 15, 30 and 50 wt%), followed by cross-linking at 180 °C and pyrolysis in argon at temperatures ranging from 1000 °C to 1500 °C. The polymer-to-ceramic transformation of the iron-modified polysilsesquioxane and the evolution at high temperatures of the synthesized SiFeOC-based nanocomposite were studied by means of thermogravimetric analysis (TGA) coupled with evolved gas analysis (EGA) as well as X-ray diffraction (XRD). Upon pyrolysis at 1100 °C, the non-modified polysilsesquioxane converts into an amorphous SiOC ceramic; whereas the iron-modified precursors lead to Fe3Si/SiOC nanocomposites. Annealing of Fe3Si/SiOC at temperatures exceeding 1300 °C induced the crystallization of Fe5Si3 and β-SiC. The crystallization of the different iron-containing phases at different temperatures is considered to be a consequence of the in situ generation of a Fe–C–Si alloy within the materials during pyrolysis. Depending on the Fe and Si content in the alloy, either Fe3Si and graphitic carbon (at 1000–1200 °C) or Fe5Si3 and β-SiC (at T > 1300 °C) crystallize. All SiFeOC-based ceramic samples were found to exhibit soft magnetic properties. Magnetization versus applied field measurements of the samples show a saturation magnetization up to 26.0 emu/g, depending on the Fe content within the SiFeOC-based samples as well as on the crystalline iron silicide phases formed during pyrolysis.  相似文献   

14.
《Ceramics International》2022,48(14):20168-20175
To improve the electromagnetic (EM) wave absorption performance of rare earth silicate in harsh environments, this work synthesized dense SiC–Y2Si2O7 composite ceramics with excellent EM wave absorption properties by using the polymer permeation pyrolysis (PIP) process, which introduced carbon and SiC into a porous Y2Si2O7 matrix to form novel composite ceramics. SiC–Y2Si2O7 composite ceramics with different numbers of PIP cycles were tested and analysed. The results show that the as-prepared composites exhibit different microstructures, porosities, dielectric properties and EM wave absorption properties. On the whole, the SiC–Y2Si2O7 composite ceramics (with a SiC/C content of 29.88 wt%) show superior microwave absorption properties. The minimum reflection loss (RLmin) reaches ?16.1 dB when the thickness is 3.9 mm at 9.8 GHz. Moreover, the effective absorption bandwidth (EAB) included a broad frequency from 8.2 GHz to 12.4 GHz as the absorbent thickness varied from 3.15 mm to 4.6 mm. In addition, the EM wave absorption mechanism was analysed profoundly, which ascribed to the multiple mediums of nanocrystalline, amorphous phases and turbostratic carbon distributed in the Y2Si2O7 matrix. Therefore, SiC–Y2Si2O7 composite ceramics with high-efficiency EM wave absorption performance promise to be a novel wave absorbing material for applications in harsh environments.  相似文献   

15.
Monophasic mullite precursors with composition of 3Al2O3·2SiO2 (3:2) were synthesized and then were sintered by Spark Plasma Sintering (SPS) to form transparent mullite ceramics. The precursor powders were calcined at 1100 °C for 2 h. The sintering was carried out by heating the sample to 1450 °C, holding for 10 min. The sintered body obtained a relative bulk density of above 97.5% and an infrared transmittance of 75–82% in wavelength of 2.5–4.3 μm without any additive. When the precursor powders were calcined at below 1100 °C, it was unfavorable for completely eliminating the residual OH, H2O and organic compound. However, when calcined temperature was too high, it was unfavorable either for full densification due to the absence of viscous flow of amorphous phase. At the same calcined temperature, the transmittance of sintered body was decreased with the increase of the sintering temperature above 1450 °C owing to the elongated grain growth.  相似文献   

16.
Using CaO, Y2O3, Al2O3, and SiO2 micron-powders as raw materials, CaO–Y2O3–Al2O3–SiO2 (CYAS) glass was prepared using water cooling method. The coefficient of thermal expansion (CTE) of CYAS glass was found to be 4.3 × 10?6/K, which was similar to that of SiCf/SiC composites. The glass transition temperature of CYAS glass was determined to be 723.1 °C. With the increase of temperature, CYAS glass powder exhibited crystallization and sintering behaviors. Below 1300 °C, yttrium disilicate, mullite and cristobalite crystals gradually precipitated out. However, above 1300 °C, the crystals started diminishing, eventually disappearing after heat treatment at 1400 °C. CYAS glass powder was used to join SiCf/SiC composites. The results showed that the joint gradually densified as brazing temperature increased, while the phase in the interlayer was consistent with that of glass powder heated at the same temperature. The holding time had little effect on phase composition of the joint, while longer holding time was more beneficial to the elimination of residual bubbles in the interlayer and promoted the infiltration of glass solder into SiCf/SiC composites. The joint brazed at 1400 °C/30 min was dense and defect-free with the highest shear strength of about 57.1 MPa.  相似文献   

17.
Oxide-bonded porous SiC ceramic filter supports were prepared using SiC powder (d50 = 212 µm), Al2O3, and clay as bond forming additives and graphite as pore former following reaction bonding of powder compacts at 1400°C in air. Reaction bonding characteristics, phase composition, porosity, pore size, mechanical strength, and microstructure of porous SiC ceramic supports were investigated. Mullite bond phase formation kinetics was studied following the Johnson–Mehl–Avrami–Kolmogorov (JMAK) model using non-isothermal differential thermal analysis (DTA) data. Compared to porous SiC ceramic filter supports having no needle-like mullite bond phase, materials processed by the mullite bonding technique exhibited higher average strength (22.1%) and elastic modulus (5.4%) at a similar porosity level of ~38%, with upper and lower bounds of their strength, modulus, and porosity being 39.1 MPa, 40.2 GPa, and 36.3% and 34.2 MPa, 31.3 GPa, and 33.0%, respectively. Spray coating method was applied for preparation of oxidation-bonded SiC filtration layer having thickness of ~150 µm and pore size of ~5–20 µm over the porous SiC support compacts using aqueous slurry made of fine SiC powder (d50 = 15 µm) followed by sintering. The layered ceramics thus prepared are potential materials for gas filter applications.  相似文献   

18.
A comparative study of the corrosion properties of thermally sprayed ceramic coatings (Al2O3, Al2O3–TiO2 with different ratios, mullite, and ZrSiO4) and their sintered bulk ceramic counterparts was performed. The coatings were deposited on corrosion-resistant steel substrates using atmospheric plasma spraying (APS) and high velocity oxy-fuel (HVOF) spraying processes. The corrosion properties were investigated in 1 N solutions of NaOH and H2SO4 at 85 °C, respectively. The coating microstructures and phase compositions, as well as the corrosive environment were shown to have a strong effect on the corrosion resistance of the coatings. Al2O3–coatings were more sensitive to these factors than Al2O3–TiO2 coatings were.The corrosion resistance of the bulk ceramics was superior to that of the thermally sprayed coatings. This is mainly because the coatings exhibited specific microstructure and contained amorphous and/or metastable phases not appearing in the bulk ceramics.  相似文献   

19.
The oxidation behaviour of AlN–SiC–TiB2 composite materials with 2, 5 and 10 mass% TiB2 and 3 mass% Fe additive obtained using powder metallurgy methods was studied in air up to 1500 °C by thermogravimetry (TG) and differential thermal analysis (DTA) techniques. The phase composition and structure of the oxide films formed were investigated using metallography, X-ray diffraction (XRD) and electron probe microanalysis (EPMA) methods. The two-stage character of non-isothermal oxidation kinetics (heating rate of 15 grade/min) of composites was established. During the first oxidation stage (up to 1350 °C), the formation of α-Al2O3, TiO2 (rutile), B2O3 and β-cristobalite as well as different aluminium borates was found. They formed as a result of interaction between Al2O3 and melted B2O3. During the second stage (above 1350–1400 °C), the mullite 3Al2O3·2SiO2 proved to be a main oxidation product in the scale; besides, some amounts of β-Al2TiO5 were formed as well. The iron additive dissolved in the mullite and aluminium titanate phases that led to the stabilization of a scale formed. It was established that for the three different TiB2 contents, oxidation isotherms follow the parabolic or paralinear rate law. The slope change on the Arrhenius plot given by the dependence of the parabolic rate constants on the reciprocal temperature, suggests a change of the oxidation mechanism in the temperature range of 1300–1350 °C. For example, for the (AlN–SiC)–5% TiB2 composite specimen, the calculated values of apparent activation energy are equal to 285 kJ/mol (1100–1300 °C) and 500 kJ/mol (1350–1550 °C), respectively. The AlN–SiC–TiB2 ceramics developed here can be recommended as high-performance materials for a use in oxidizing medium up to 1450 °C.  相似文献   

20.
A commercial silicone resin (“silicone”) filled with ceramic nanoparticles has been employed for the preparation of mullite and β-SiAlON ceramics. Dense, pure, crack free mullite were prepared by the heating in air of a mixture of silicone resin and alumina nanoparticles in the temperature range 1200–1550 °C. The high reactivity of Al2O3 towards silica, coupled with nanometric size, led to a large volume fraction of mullite crystals even at low firing temperatures (1250 °C). β-SiAlON ceramics were prepared by the heating of a mixture of silicone resin and fillers consisting of Al2O3 nanoparticles and Si3N4 and AlN microparticles, in the temperature range 1450–1550 °C in nitrogen atmosphere. The formation of SiAlON was found to be preceded by the formation of intermediate alumino-silicate phases like mullite and sillimanite, successively reduced (due to the carbon content of the ceramic residue of silicone resins) and nitrided. Although some oxide contamination was still present after the high temperature treatment, a high β-SiAlON yield (about 80%) was achieved. The use of nano-filled silicones provides a promising route for the fabrication of advanced ceramic components by exploiting polymer processing techniques, with the achievement of complex shapes.  相似文献   

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