Spheroidization of SiC powders and their improvement on the properties of SiC porous ceramics

Spherical SiC powders were prepared at high temperature using commercial SiC powders (4.52 µm) with irregular morphology. The influence of spherical SiC powders on the properties of SiC porous ceramics was investigated. In comparison with the as-received powders, the spheroidized SiC powders exhibited a relatively narrow particle size distribution and better flowability. The spheroidization mechanism of irregular SiC powder is surface diffusion. SiC porous ceramics prepared from spheroidized SiC powders showed more uniform pore size distribution and higher bending strength than that from as-received SiC powders. The improvement in the performance of SiC porous ceramics from spheroidized powder was attributed to tighter stacking of spherical SiC particles. After sintering at 1800 °C, the open porosity, average pore diameter, and bending strength of SiC porous ceramics prepared from spheroidized SiC powder were 39%, 2803.4 nm, and 66.89 MPa, respectively. Hence, SiC porous ceramics prepared from spheroidized SiC powder could be used as membrane for micro-filtration or as support of membrane for ultra/nano-filtration.     

Spheroidization of low-cost alumina powders for the preparation of high-flux flat-sheet ceramic membranes

Two kinds of low-cost alumina powders with irregular morphology were pretreated by spheroidization and the two spherical powders were used to prepare high-flux flat-sheet support and microfiltration (MF) membrane with high separation accuracy, respectively. It was found that the spheroidization pretreatment not only unified the morphology of alumina powder particles into spherical shape, but also narrowed the particle size distribution of the powders, which both were conducive to optimizing the performance of the as-prepared ceramic membranes. After sintering at 1350 °C, the open porosity, bending strength, average pore diameter and pure water permeability of alumina flat-sheet support from spheroidized alumina coarse powder were 44.3%, 36.3 MPa, 3.3 μm and 3240 L/h m² bar, respectively. The slurry derived from spheroidized alumina fine powder was dip-coated on the flat-sheet support to prepare MF membrane. The crack-free MF membrane with a thickness of 23.5 μm had a pore diameter of 0.12 μm and pure water permeability of 850 L/h m² bar. Additionally, the elaborated MF membrane was used to clarify aqueous suspension of carbon black with the maximum rejection rate of up to 99.7%, exhibiting excellent cleaning performance at the same time by completely restore the virgin permeate flux after backwash.     

ρ-Al2O3添加量对原位反应结合碳化硅膜支撑体性能的影响

以黑色碳化硅为骨料,添加不同含量的ρ-Al2O3,在1430℃、无压条件下,用碳化硅表面氧化产生的SiO2与Al2O3反应制备多孔碳化硅膜支撑体,研究了ρ-Al2O3添加量对碳化硅支撑体粘结相组成及性能的影响。结果表明,ρ-Al2O3添加量由3wt%增加到15wt%时,试样烧结后粘结相中莫来石相增多,石英相减少但不能完全消除,支撑体的显气孔率降低,孔径减小,透气度由1127.8 m3?cm/(m2?h?kPa)下降到210.4 m3?cm/(m2?h?kPa);支撑体抗弯强度先增大后降低,ρ-Al2O3添加量为9wt%时,支撑体抗弯强度为25.1 MPa,透气度为372.7 m3?cm/(m2?h?kPa),支撑体的综合性能满足高温含尘气体过滤的要求。     

Preparation processes and characterizations of alumina-coated alumina support layers and alumina-coated natural material-based support layers for microfiltration

Recently, porous ceramic membranes have become a subject of significant interest due to their outstanding thermal and chemical stability. To reduce the high manufacturing costs of these porous ceramic membranes, recent research has focused on the utilization of inexpensive natural materials. However, there have not been any well-established direct comparisons of the membrane properties between typical alumina-based membranes and novel natural material-based membranes. Therefore, we compared alumina-coated alumina support layers (with average pore sizes ranging from 0.10 µm ~0.18 µm), alumina-coated diatomite-kaolin composite support layers (with an average pore size of 0.12 µm), and alumina-coated pyrophyllite-diatomite composite support layers (with an average pore size of 0.11 µm) via the dip-coating method and subsequent heat treatment ranging from 1200 °C–1400 °C for 1 h. The pure water permeability of the alumina-coated diatomite-kaolin composite support layer and the alumina-coated pyrophyllite-diatomite composite support layer was found to be approximately 2.0×10² L m⁻² h⁻¹ bar⁻¹, which is similar to that of an alumina-coated alumina support layer. Therefore, we suggest that the average pore size of an alumina-coated natural material-based support layer can be effectively controlled while exhibiting acceptable water permeability.     

The membrane properties of alumina-coated alumina support layers and alumina-coated diatomite–kaolin composite support layers

ABSTRACT

Porous ceramic membranes are a current research focus because of their outstanding thermal and chemical stability. Recent research has utilised inexpensive natural materials such as diatomite to reduce the expense of these porous ceramic membranes. However, insufficient data exist for microfiltration applications using the diatomite-based membranes. The measured membrane properties of alumina-coated alumina support layers and alumina-coated diatomite–kaolin composite support layers have been compared. These experiments have been used to determine whether the average pore size could be reduced effectively by controlling the thickness of the alumina coating layer, while maintaining acceptable water permeability. The membrane properties of the alumina-coated alumina support layers and the alumina-coated diatomite–kaolin composite support layers were examined using the scanning electron microscopy, mercury porosimetry, and a dead-end microfiltration system.     

Design and fabrication of whisker hybrid ceramic membranes with narrow pore size distribution and high permeability via co-sintering process

Ceramic microfiltration membranes (MF) with narrow pore size distribution and high permeability are widely used for the preparation of ceramic ultrafiltration membranes (UF) and in wastewater treatment. In this work, a whisker hybrid ceramic membrane (WHCM) consisting of a whisker layer and an alumina layer was designed to achieve high permeability and narrow pore size distribution based on the relative resistance obtained using the Hagen-Poiseuille and Darcy equations. The whisker layer was designed to prevent the penetration of alumina particles into the support and ensure a high porosity of the membrane, while the alumina layer provided a smooth surface and narrow pore size distribution. Mass transfer resistance is critical to reduce the effect of the membrane layers. It was found that the resistance of the WHCM depended largely on the alumina layer. The effect of the support and whisker layer on the resistance of the WHCM was negligible. This was consistent with theoretical calculations. The WHCM was co-sintered at 1000?°C, which resulted in a high permeability of ~?645?L?m^?1 h^?1 ;bar^?1 and a narrow pore size distribution of ~?100?nm. Co-sintering was carried out on a macroporous ceramic support (just needed one sintering process), which greatly reduced the preparation cost and time. The WHCM (as the sub-layer) also showed a great potential to be used for the fabrication of ceramic UF membranes with high repeatability. Hence, this study provides an efficient approach for the fabrication of advanced ceramic MF membranes on macroporous supports, allowing for rapid prototyping with scale-up capability.     

Synthesis of Nanoparticulate Silica Composite Membranes by the Pressurized Sol–Gel Technique

A crack-free silica composite membrane has been synthesized from a nanoparticulate silica sol (particle diameter <10 nm) by a pressurized sol–gel coating technique developed in this study. The microporous silica layers with an estimated pore radius of 0.78 nm were deposited inside the pores (average pore size of 0.1 μm) of slip cast a-alumina support tubes. The microstructure of the coated layer was controlled by adjusting sol properties and pressurizing conditions. The room-temperature intrinsic permeability of N₂ through the silica membrane layer after heat treatment at 200°C is about 4.9 × 10⁻¹² mol·m/m²·s· Pa, and the mechanism of gas transport is Knudsen flow. The thermal stability of the silica composite membrane is excellent up to 500°C.     

Reaction-bonded robust SiC ceramic membranes sintered at low temperature with coal gangue

Herein, we report an in-situ reaction-bonded SiC membrane sintered at low temperature using a solid waste (i.e. coal gangue) as the sintering aid to form strong neck connections. The effects of sintering temperature and coal gangue proportion on their properties regarding pore size, open porosity, bending strength and pure water permeability were investigated. The single-channel tubular SiC membrane sintered at 1300 °C with a coal gangue proportion of 12 wt% was optimal, exhibiting an average pore size of 2.78 μm, a open porosity of 47.08%, a bending strength of 34.01 ± 1.3 MPa and a high water permeability of 83967 L m⁻² h⁻¹ bar⁻¹. The membrane could completely reject D₅₀ = 0.87 μm SiC solids and presented a steady-state water permeability of 458 L m⁻² h⁻¹·bar⁻¹. The SiC membrane could be regenerated through ultrasonication and its steady-state water permeability was almost unchanged for 3 cycles, proving its mechanical robustness. This work may appeal to the practical low-cost production of high-performance SiC membranes.     

Evaporation-condensation derived silicon carbide membrane from silicon carbide particles with different sizes

Silicon carbide ceramic is a promising membrane material because of the high corrosive and high temperature resistance, and the excellent hydrophility. Here, a silicon carbide ceramic membrane with both substrate layer and separate layer composed of pure silicon carbide phase was successfully prepared. The effect of particle size on the microstructure and properties was investigated. The substrates were prepared from three silicon carbide particles at 2200 ℃. With the content increase of fine particle, the average pore size increased from 5.6 μm to 14.1 μm; meanwhile, the flexural strength of the substrate increased from 14.1 MPa to 24.6 MPa. The separation layers were made from particles of 3.0 μm and 0.5 μm. When sintered at 1900 ℃, the separation layer formed pore network with homogeneous structure. Such silicon ceramic membrane can be used in harsh conditions, including high temperature wastewater and strongly corrosive wastewater.     

Oxidation bonding of porous silicon carbide ceramics with synergistic performance

Porous silicon carbide (SiC) ceramics were fabricated by an oxidation-bonding process, in which the powder compacts are heated in air so that SiC particles are bonded to each other by oxidation-derived SiO₂ glass. It has been shown that a high porosity can be obtained by adding a large amount of graphite into the SiC powder compacts and that the pore diameter can be controlled by the size of graphite particles and/or SiC powders. When a 0.3-μm SiC powder was used, a high strength up to 133 MPa was achieved at a porosity of 31.5%. Moreover, oxidation-bonded SiC (OBSC) ceramics were observed to exhibit an excellent resistance to oxidation and thermal shock.     

Effect of SiC powder on the properties of SiC slurry for stereolithography

Silicon carbide (SiC) is a kind of structural ceramics with excellent properties and it is widely used in industrial fields. Stereolithography (SL) is a potential additive manufacturing technique to fabricate fine complex SiC components, the resin-based SiC slurry with superior rheological and photo-polymerization properties is important for SL. In this paper, we investigated the influence of SiC powder on the properties of the SiC slurries for SL. The physical characteristics of SiC powder such as particle size, size distribution and appearance were tested and observed, and their influence on the dispersion, sedimentation and photo-polymerization property of the SiC slurry were investigated and discussed in detail based on their correlative theory, we finally prepared SiC slurry with superior rheological and photo-polymerization properties, and fabricated the fine complex SiC green body with low defects, high accuracy and high bending strength successfully. The SiC slurry with the solid content of 40 vol% was fabricated by the SiC powder with the median diameter D₅₀ ≈ 10.0 μm and a narrow particle size distribution, it is Bingham fluid with good fluidity and the viscosity of it is 464.40 mPa s under the shear rate of 51.08 s^?1, the cured SiC parts with Z – axis dimension change of 0.75% was finally fabricated, the three points bending strength of it is 50.18 MPa. Our research work provides some fundamental understanding of the SL technique for fabricating fine complex SiC components, explored a suitable way to fabricate high quality SiC green parts through SL, and offers some valuable references for preparing SiC slurry with superior rheological and photo-polymerization properties.     

颗粒粒径和膜孔径对陶瓷膜微滤微米级颗粒悬浮液的影响

通过测定颗粒悬浮液通过陶瓷微滤膜时的参透通量及污染阻力,确定了陶瓷膜处理微米级颗粒悬浮液时,颗粒粒径和膜孔径对微滤过程的影响和膜污染机理,获得了微米级颗粒悬浮液微滤过程中膜孔径的选择方法。     

Deposition of thin ultrafiltration membranes on commercial SiC microfiltration tubes

Porous SiC based materials present high mechanical, chemical and thermal robustness, and thus have been largely applied to water-filtration technologies. In this study, commercial SiC microfiltration tubes with nominal pore size of 0.04 μm were used as carrier for depositing thin aluminum oxide (Al₂O₃) ultrafiltration membranes. These ultrafiltration membranes were obtained by coating, drying and calcination of a colloidal suspension of boehmite particles. After calcination, the membrane material consisted of nanosized γ-Al₂O₃ crystallites and had a narrow pore size distribution with average pore size of 5.5 nm. Membrane thickness was tuned by repeating the coating of boehmite sol. By doing so, we were able to reduce the defect density on the membrane surface, as evidenced by SEM analysis and by the significant reduction of water permeance after depositing the second γ-Al₂O₃ layer. After five times coating, a 5.6 µm thick γ-Al₂O₃ layer was obtained. This membrane shows retention of ~75% for polyethylene glycol molecules with M_n of 8 and 35 kDa, indicating that, despite their intrinsic surface roughness, commercial SiC microfiltration tubes can be applied as carrier for thin ultrafiltration membranes. This work also indicates that an improvement of the commercial SiC support surface smoothness may greatly enhance permeance and selectivity of γ-Al₂O₃ ultrafiltration membranes by allowing the deposition of thinner defect-free layers.     

A hybrid graphite powder PFC@G for reserving higher carbon content of self-lubrication graphite/SiC composites by RMI

The appropriate carbon content is indispensable for the application of self-lubricating graphite/SiC composites. However, it is a big challenge to retain high carbon content in the reaction-formed graphite/SiC composites because of drastic consumption of carbon by violent reaction with liquid silicon. In this study, a hybrid powder constructed by graphite particles (G) and glassy carbon derived from phenolic resin (PFC) was used as carbon sources, or PFC@G for short, to reserve higher content of carbon in the reaction-formed composites. The weight ratio of phenolic resin to graphite particles was adjusted to obtain an appropriate PFC@G with dense microstructure and close-grained surface. Compared with the graphite/SiC composites only using raw graphite particles as carbon sources, the carbon content of the composites fabricated with compact and large PFC@G has obviously increased (up to 172%). In particular, the carbon content of the composites fabricated with the weight ratio = 0.8 reached a high value of 44.26 vol.%, which exhibited outstanding self-lubrication properties among the four kinds of the composites. The mechanism of reserving higher content of carbon in the graphite/SiC composites by constructing PFC@G is investigated, revealing that a continuous SiC layer formed on the surface of the larger size PFC@G and most closely packed graphite particles inside of PFC@G were insulate from liquid silicon by the layer.     

Microstructure and properties of porous SiC ceramics by LPCVI technique regulation

A new gradient pore structure in porous SiC ceramics was fabricated by low pressure chemical vapor infiltration (LPCVI). Effects of deposition duration on the mechanical properties and permeability of porous SiC ceramics were investigated. Results demonstrated that pore diameter and shapes decreased from the surface to the interior along with LPCVI duration. Porous SiC ceramics with deposition duration of 160 h exhibited flexural strength of 48.05 MPa and fracture toughness of 1.30 MPa m^1/2, where 221% and 189% improvements were obtained compared to porous SiC ceramics without LPCVI, due to CVI-SiC layer strengthening effect. Additionally, at the same gas velocity, pressure drop increase rate was faster due to apparent porosity and pore size change.     

Microstructural Characterization of Porous Silicon Carbide Membrane Support With and Without Alumina Additive

Porous silicon carbide (SiC) membrane supports sintered at 1500°–1800°C were prepared by cold isostatic pressing (CIP) under different pressures and using different amounts of alumina additive (0%–4%). The relationship between processing factors and pore size and microstructure was examined. Varying the sintering temperature, the CIP pressure and the amount of additive used were found to be effective for controlling pore size and microstructure. The pore size and particle size of the membrane support prepared without alumina were found to increase with increasing sintering temperature. This was attributed to surface diffusion. Densification of the undoped support did not occur, however, because of concurrent pore development. In the SiC membrane support containing 4% alumina, small particles and a pore size of around 100 nm were retained. This was because of the formation of a limited amount of SiO₂–Al₂O₃ liquid phase during sintering.     

High-flux whisker layer ceramic membrane prepared by gel spin-coating method for low-pressure oil/water emulsion filtration

Insufficient permeability and membrane fouling significantly influence the efficiency of ceramic microfiltration (MF) membranes in oil/water emulsion treatment. In this study, a high-flux whisker layer ceramic MF membrane with super-hydrophilicity was successfully fabricated through gel-spin coating method and a low-temperature oxidation method, which was used to separate oil/water emulsion. The effects of the whisker layer and surface wettability were systematically investigated, and the mechanism of in-situ gelling and pore size distribution was proposed. The super-hydrophilic ceramic MF membrane with an average pore size of 250 nm exhibited a high gas flux of 934 m³/(m²·h·bar) and excellent pure water flux of 9754 L/(m² h bar). Even after a long-term circulating filtration process, the super-hydrophilic ceramic MF membrane still maintained a high water flux of over 50 L/(m²·h) at a transmembrane pressure of 5 KPa during the treatment of oil-in-water emulsion with a concentration of 1000 mg/L. Overall, the developed ceramic MF membrane demonstrated high permeability and excellent anti-fouling performance, making it a promising candidate for oil/water emulsion wastewater treatment.     

Evaluation of Air Permeation Behavior of Porous SiC Ceramics Synthesized by Oxidation‐Bonding Technique

Porous SiC ceramics were synthesized by oxidation bonding of compacts of commercial α‐SiC powder at 1300°C. Different volume fractions of petroleum coke powder were used for variation of porosity of ceramics from 36% to 56%. The material exhibited variations of pore size from 3 to 15 μm, flexural strength from 5.5 to 29.5 MPa, and elastic modulus from 3.3 to 27.6 GPa. Air permeation behavior was studied at 26–650°C. At room temperature Darcian (k₁) and non‐Darcian (k₂) permeability parameters vary from 1.64 to 18.42 × 10^?13 m² and 0.58 to 2.95 × 10^?7 m, respectively. Temperature dependence of permeability was explained from structural changes occurring during test conditions.     

Studies on processing of layered oxide-bonded porous sic ceramic filter materials

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.     

Processing and properties of glass-bonded silicon carbide membrane supports

Porous SiC membrane supports were fabricated from SiC and glass frit at a temperature as low as 850 °C in air by a simple pressing and heat-treatment process. The effects of the initial SiC particle size and frit content on the porosity, flexural strength, and air permeation of the membrane supports were investigated. During heat-treatment, the glass frit transformed to a viscous glass phase, which acted as a bonding material between SiC particles and as a protecting layer for severe oxidation of SiC particles. The porosity of the porous SiC membrane supports could be controlled within a range of 37–46% with the present set of processing conditions. The typical flexural strength, permeability, and specific air flow rate of the porous membrane supports fabricated using 23 μm SiC particles with 15 wt% glass frit were 75 MPa, 4.2 × 10⁻¹³ m², and 32.4 L/min/cm², respectively.