CN105669207B - A kind of SiC Mo4.8Si3C0.6The preparation method of composite - Google Patents

A kind of SiC Mo4.8Si3C0.6The preparation method of composite Download PDF

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CN105669207B
CN105669207B CN201610060119.7A CN201610060119A CN105669207B CN 105669207 B CN105669207 B CN 105669207B CN 201610060119 A CN201610060119 A CN 201610060119A CN 105669207 B CN105669207 B CN 105669207B
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preparation
mixed solution
ludox
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CN105669207A (en
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曹丽云
白喆
黄剑锋
欧阳海波
李翠艳
孔新刚
费杰
卢靖
王程
李嘉胤
介燕妮
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Shaanxi University of Science and Technology
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    • C04B35/56Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides
    • C04B35/565Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides based on silicon carbide
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    • C04B35/58Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides
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Abstract

A kind of SiC Mo4.8Si3C0.6The preparation method of composite, ammonium paramolybdate is added in glucose solution, fully after dissolving; add Ludox and be well mixed; 12~36h of hydro-thermal reaction is carried out in 160~200 DEG C, then 2~4h of heat treatment is carried out under 1350~1550 DEG C of argon gas atmospheres are protected, finally gives SiC Mo4.8Si3C0.6Composite.Composite density prepared by the present invention is moderate, and particle size is small, has good high-temperature oxidation resistance.Raw material of the present invention is readily available, and preparation technology is simple, easy to operate, and cost is low, environment-friendly pollution-free.

Description

A kind of SiC-Mo4.8Si3C0.6The preparation method of composite
Technical field
The invention belongs to field of material preparation, and in particular to a kind of SiC-Mo4.8Si3C0.6The preparation method of composite.
Background technology
It is corrosion-resistant due to high-melting-point, the excellent resistance to elevated temperatures such as anti-oxidant, not available for medium density and other materials Other performances, compound is widely used in the key areas such as civilian and national defence between silicon molybdenum.Such as molybdenum disilicide (MoSi2) Have been used for antioxidant coating and high temperature exothermic body material;Molybdenum silicide (Mo5Si3) have in terms of high-temperature structural material it is huge Big application prospect.Mo4.8Si3C0.6There is high-melting-point as a kind of Mo-Si-C ternary phases chemicals are similar to silicon molybdenum compound, Moderate density, preferable high-temperature oxidation resistance, high-temperature structural material and high-temperature oxidation-resistant material can be used as, is got a good eye Value, but at present for Mo4.8Si3C0.6Research it is less, and progress is relatively slow.
Mo4.8Si3C0.6It can be stabilized higher than 1300 degrees Celsius, there is document report to claim, Mo4.8Si3C0.6C under high temperature, MoSi2Unique existing stable phase between SiC three-phases.Usual Mo4.8Si3C0.6It is by Mo5Si3At high temperature gradually transformation and Come.B.A.Gnesin and I.B.Gnesin et al. are by mixing Mo5Si3After powder and the mixing of carbon or diamond dust, in argon Under gas atmosphere protection [Gnesin B A, Gnesin I B.Synthesis of are formed in 1750-1850 DEG C by two-step sintering the Nowotny phase Mo4.8Si3C0.6from Mo5Si3+carbon mixtures[J].Inorganic Materials,2015, 51(10):991-998.].Qingshan Zhu, Kazuhisa Shobu et al. passes through mixing and ball milling MoSi2, SiC, Mo powder, with 2100 DEG C of lower reactions of argon gas atmosphere protection after drying, it is cooled to 1000 DEG C afterwards with given pace [Zhu Q,Shobu K,Tani E,et al.High‐Temperature Strength and Creep Behavior of Melt‐Infiltrated SiC-Mo≤5Si3C≤1 Composites[J].Journal of the American Ceramic Society,2004,82(8):2276-2278.].Suzuki Y, Niihara K. are also prepared except Mo- by hot pressure reaction Si-C ternary phases [Suzuki Y, Niihara K.Synthesis and mechanical properties of Mo 5Si3C≤1and Mo≤5Si3C≤1-based composites[J].Intermetallics,1998, 6(1):7-13.]。
Mo prepared by above method≤5Si3C≤1Compound needs the reaction condition of higher reaction temperature or harshness, Ask high, step is numerous and diverse, efficiency is low, is unfavorable for industrialized production.
The content of the invention
The defects of in order to overcome above-mentioned prior art to exist, it is an object of the invention to provide a kind of SiC-Mo4.8Si3C0.6 The preparation method of composite, this method reaction temperature is relatively low, simple to operate, and repeatability is high, by the SiC- of party's legal system Mo4.8Si3C0.6Composite has certain good high-temperature behavior.
To achieve these goals, the present invention uses following technical scheme.
A kind of SiC-Mo4.8Si3C0.6The preparation method of composite, comprises the following steps:
1) ammonium paramolybdate is added in D/W, stirs to ammonium paramolybdate and be completely dissolved, obtain mixed solution; The addition of ammonium paramolybdate and the ratio of D/W are (0.2~0.5) g:(30~40) mL;
2) Ludox is added into mixed solution, after stirring, at 160~200 DEG C carry out hydro-thermal reaction 12~ 36h, after reaction terminates, reacting liquid filtering is precipitated, and dried;
3) by it is dried precipitation be placed in vacuum drying oven, argon gas protection under at 1350~1550 DEG C heat treatment process 2 ~4h, obtains SiC-Mo4.8Si3C0.6Composite.
The concentration of D/W is 0.1~0.2mol/L in step 1).
The silica quality fraction of Ludox is 10~20% in step 2).
The ratio of mixed solution and Ludox is (30~40) mL in step 2):(2~10) mL.
Stirred in step 2) is realized by 2~5h of magnetic agitation.
Drying is 4~8h of drying at 60~100 DEG C in step 2).
Water heating kettle packing volume ratio is 30~50% during step 2) hydro-thermal reaction.
Compared with prior art, the invention has the advantages that:
Preparation method provided by the invention is using ammonium paramolybdate as molybdenum source, and glucose is carbon source, and Ludox is silicon source, through filling Divide after being stirred, hydrothermal crystallization reaction is carried out at 160~200 DEG C, is heat-treated then at 1350~1550 DEG C, final system Obtain SiC-Mo4.8Si3C0.6Composite;Reaction condition of the present invention is gentle, and required temperature is relatively low, and processing step is simple, weight Renaturation is high, is advantageous to industrialized production, and the product prepared has higher purity., can be clear by XRD diffracting spectrums Reflect by SiC-Mo produced by the present invention4.8Si3C0.6Composite is by SiC and Mo4.8Si3C0.6Composition, without other dephasigns; By stereoscan photograph as can be seen that the composite material powder pattern is irregular, it is divided into spherical and sheet, and particle size It is small.
Brief description of the drawings
Fig. 1 is SiC-Mo prepared by the present invention4.8Si3C0.6The X-ray diffraction XRD spectrum of composite;
Fig. 2 is SiC-Mo prepared by the present invention4.8Si3C0.6The scanning electron microscope sem photo of composite.
Embodiment
Below in conjunction with the accompanying drawings and specific embodiment is described in further detail to the present invention:
Embodiment 1
A kind of SiC-Mo4.8Si3C0.6The preparation method of composite, comprises the following steps:
1) 0.28g ammonium paramolybdates are added in 40mL 0.1mol/L D/W, are stirred well to secondary molybdenum Sour ammonium is completely dissolved, and obtains mixed solution;
2) Ludox that 5mL silica quality fraction is 20% is added into above-mentioned mixed solution, and (manufacturer is mountain Eastern hundred special new material Co., Ltds), after magnetic agitation 2h, hydro-thermal reaction 12h are carried out in 180 DEG C, after reaction terminates, by reaction solution It is filtrated to get precipitation;Water heating kettle packing volume ratio is 50% during hydro-thermal reaction;
3) after precipitation is scrubbed, 4h is dried in 60 DEG C of vacuum drying chambers;
4) dried precipitation is placed in vacuum drying oven, 1500 DEG C of heat treatment process 3h under argon gas protection, finally given SiC-Mo4.8Si3C0.6Composite.
Embodiment 2
A kind of SiC-Mo4.8Si3C0.6The preparation method of composite, comprises the following steps:
1) 0.5g ammonium paramolybdates are added in 30mL 0.2mol/L D/W, are stirred well to para-molybdic acid Ammonium is completely dissolved, and obtains mixed solution;
2) it is 10% Ludox 10mL silica quality fraction to be added into above-mentioned mixed solution, after magnetic agitation 4h, Hydro-thermal reaction 36h is carried out in 200 DEG C, after reaction terminates, reacting liquid filtering is precipitated;Water heating kettle is filled during hydro-thermal reaction Volume ratio is 40%;
3) after precipitation is scrubbed, 2h is dried in 100 DEG C of vacuum drying chambers;
4) dried precipitation is placed in vacuum drying oven, 1550 DEG C of heat treatment process 2h under argon gas protection, finally given SiC-Mo4.8Si3C0.6Composite.
Embodiment 3
A kind of SiC-Mo4.8Si3C0.6The preparation method of composite, comprises the following steps:
1) 0.32g ammonium paramolybdates are added in 35mL 0.15mol/L D/W, are stirred well to secondary molybdenum Sour ammonium is completely dissolved, and obtains mixed solution;
2) 3mL silica quality fraction is added into above-mentioned mixed solution as 15% Ludox, after magnetic agitation 3h, Hydro-thermal reaction 12h is carried out in 200 DEG C, after reaction terminates, reacting liquid filtering is precipitated;Water heating kettle is filled during hydro-thermal reaction Volume ratio is 30%;
3) after precipitation is scrubbed, 4h is dried in 60 DEG C of vacuum drying chambers;
4) dried precipitation is placed in vacuum drying oven, 1400 DEG C of heat treatment process 4h under argon gas protection, finally given SiC-Mo4.8Si3C0.6Composite.
Embodiment 4
A kind of SiC-Mo4.8Si3C0.6The preparation method of composite, comprises the following steps:
1) 0.4g ammonium paramolybdates are added in 40mL 0.1mol/L D/W, are stirred well to para-molybdic acid Ammonium is completely dissolved, and obtains mixed solution;
2) 8mL silica quality fraction is added into above-mentioned mixed solution as 15% Ludox, after magnetic agitation 4h, Hydro-thermal reaction 36h is carried out in 160 DEG C, after reaction terminates, reacting liquid filtering is precipitated;Water heating kettle obturator during hydro-thermal reaction Product is than being 35%;
3) after precipitation is scrubbed, 3h is dried in 80 DEG C of vacuum drying chambers;
4) dried precipitation is placed in vacuum drying oven, 1350 DEG C of heat treatment process 4h under argon gas protection, finally given SiC-Mo4.8Si3C0.6Composite.
Embodiment 5
A kind of SiC-Mo4.8Si3C0.6The preparation method of composite, comprises the following steps:
1) 0.4g ammonium paramolybdates are added in 37mL 0.2mol/L D/W, are stirred well to para-molybdic acid Ammonium is completely dissolved, and obtains mixed solution;
2) it is Ludox that 6mL silica quality fraction 12% is added into above-mentioned mixed solution, after magnetic agitation 5h, in 180 DEG C of progress hydro-thermal reaction 24h, after reaction terminates, reacting liquid filtering is precipitated;Water heating kettle packing volume during hydro-thermal reaction Than for 45%;
3) after precipitation is scrubbed, 3h is dried in 100 DEG C of vacuum drying chambers;
4) dried precipitation is placed in vacuum drying oven, 1400 DEG C of heat treatment process 2h under argon gas protection, finally given SiC-Mo4.8Si3C0.6Composite.
Embodiment 6
A kind of SiC-Mo4.8Si3C0.6The preparation method of composite, comprises the following steps:
1) 0.2g ammonium paramolybdates are added in 32mL 0.12mol/L D/W, are stirred well to secondary molybdenum Sour ammonium is completely dissolved, and obtains mixed solution;
2) it is Ludox that 2mL silica quality fraction 17% is added into above-mentioned mixed solution, after magnetic agitation 3h, in 170 DEG C of progress hydro-thermal reaction 30h, after reaction terminates, reacting liquid filtering is precipitated;Water heating kettle packing volume during hydro-thermal reaction Than for 45%;
3) after precipitation is scrubbed, 8h is dried in 70 DEG C of vacuum drying chambers;
4) dried precipitation is placed in vacuum drying oven, 1450 DEG C of heat treatment process 2h under argon gas protection, finally given SiC-Mo4.8Si3C0.6Composite.
It is the SiC-Mo prepared by the present invention referring to Fig. 14.8Si3C0.6The XRD spectrum of composite.As seen from the figure: Product Mo prepared by the present invention4.8Si3C0.6With SiC compound phases, by with Mo4.8Si3C0.6Standard PDF cards (43-1199) And SiC standard card (65-0360) is compared, it was demonstrated that product SiC-Mo prepared by the present invention4.8Si3C0.6Composite wood Material.
Referring to Fig. 2, it is to prepare SiC-Mo by the present invention4.8Si3C0.6The SEM photograph of composite material powder.Can from figure Clearly to find out:The SiC-Mo that the present invention obtains4.8Si3C0.6Composite pattern is irregular, is made up of spherical and sheet, and Particle size is small.

Claims (4)

  1. A kind of 1. SiC-Mo4.8Si3C0.6The preparation method of composite, it is characterised in that comprise the following steps:
    1) ammonium paramolybdate is added in D/W, stirs to ammonium paramolybdate and be completely dissolved, obtain mixed solution;Secondary molybdenum The addition of sour ammonium and the ratio of D/W are (0.2~0.5) g:(30~40) mL;The wherein concentration of D/W For 0.1~0.2mol/L;
    2) Ludox is added into mixed solution, after stirring, 12~36h of hydro-thermal reaction is carried out at 160~200 DEG C, instead After should terminating, reacting liquid filtering is precipitated, and dried;Wherein, the silica quality fraction of Ludox is 10~20%, The ratio of mixed solution and Ludox is (30~40) mL:(2~10) mL;
    3) by it is dried precipitation be placed in vacuum drying oven, argon gas protection under at 1350~1550 DEG C 2~4h of heat treatment process, Obtain SiC-Mo4.8Si3C0.6Composite.
  2. A kind of 2. SiC-Mo according to claim 14.8Si3C0.6The preparation method of composite, it is characterised in that step 2) stirred in is realized by 2~5h of magnetic agitation.
  3. A kind of 3. SiC-Mo according to claim 14.8Si3C0.6The preparation method of composite, it is characterised in that step 2) drying is 4~8h of drying at 60~100 DEG C in.
  4. A kind of 4. SiC-Mo according to claim 14.8Si3C0.6The preparation method of composite, it is characterised in that step 2) water heating kettle packing volume ratio is 30~50% during hydro-thermal reaction.
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