CN104810065A - Cobalt-containing coated particles and preparation method thereof - Google Patents
Cobalt-containing coated particles and preparation method thereof Download PDFInfo
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- CN104810065A CN104810065A CN201510122718.2A CN201510122718A CN104810065A CN 104810065 A CN104810065 A CN 104810065A CN 201510122718 A CN201510122718 A CN 201510122718A CN 104810065 A CN104810065 A CN 104810065A
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
- G21C3/02—Fuel elements
- G21C3/04—Constructional details
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C21/00—Apparatus or processes specially adapted to the manufacture of reactors or parts thereof
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
Abstract
The invention provides design of cobalt-containing coated particles for tracing different fuel elements in reactors. The cobalt-containing coated particles adopt a multi-layer structure, and cores of the particles are cobalt-containing ceramic particles which are formed by carbide or oxide ceramic of dispersed single cobalt or a dispersed cobalt compound; the dimensions of the cores are in a range of 200-900 mu m, and the mass fraction of cobalt contained in the cores ranges from 0.1%-35%; a low-temperature coating silicon carbide layer, an inner pyrolytic carbon layer, a high-temperature coating silicon carbide layer and an outer pyrolytic carbon layer are sequentially arranged from each core to the outside. A full-ceramic multi-layer-coating cobalt-containing coated particle form is designed, and cobalt elements are constrained in the coated particles. Particularly, the low-temperature coating silicon carbide layers are used as the innermost layers of the coating layers, cobalt precipitation during coating and follow-up treatment is prevented, and effects caused by tracing particles on internal environments of the reactors under the in-reactor running condition are avoided.
Description
Technical field
The invention belongs to pellet design and field of material preparation, be specifically related to a kind of for spike containing cobalt coated particle and preparation method thereof.
Background technology
The energy is one of material motive power promoting socio-economic development, the fossil energy of current dominate has in use caused such as large area and has continued a large amount of environmental problems such as haze pollution, therefore, scientific and reasonable energy structure is set up and the problem such as to tap a new source of energy becomes more and more urgent.As the nuclear energy of clean energy resource, its investigation and application is also in a new developing stage.The operation of nuclear power station be unable to do without nuclear fuel element, and at present according to the difference of heap-type, the different fuel element of form is designed endlessly.For same heap-type, its fuel element design parameter can change, but its surface structure pattern is identical, and this just needs certain technological means to distinguish different fuel elements.Especially for New-type fuel element, in order to verify usability in its heap, often need the nuclear fuel loading amount designing different abundance or different quality to realize optimum generating efficiency, the fuel element how distinguishing different parameters becomes a problem demanding prompt solution.
Reactor inside is high radioactivity environment, and general differentiating method is difficult to operate.Utilize
59co can become in neutron irradiation environment
60co, usual loop all can be installed gamma spectrometer and detect for burnup, and
60the characteristic gamma spectrum of Co can well be detected, and this kind of method therefore can be utilized to carry out the differentiation of different fuel element in reactor.
Summary of the invention
For this area Problems existing, the object of the invention is to propose the core core containing cobalt coated particle and clad design, thus propose a kind of containing cobalt coated particle.
Another object of the present invention proposes the preparation method containing cobalt coated particle.
3rd object of the present invention proposes the described application containing cobalt coated particle.
The technical scheme realizing the object of the invention is:
A kind of containing cobalt coated particle, described have sandwich construction containing cobalt coated particle, the core core of particle is the ceramic particle containing cobalt, described ceramic particle is for matrix with oxide or carbonide, the oxide of cobalt or cobalt is dispersed in carbonide or oxide matrix, core core is of a size of 200 ~ 900 μm, and core core is 0.1% ~ 35% containing cobalt massfraction; From core core outside coated low-temperature carbonization silicon layer, internal layer pyrolysis layer of charcoal, high temperature cabonization silicon layer and outer pyrolysis layer of charcoal successively.
Further, described ceramic particle take carbonide as matrix, and in cobalt dispersed carbides matrix, cobalt massfraction in ceramic particle is 1 ~ 20%; Or described ceramic particle take oxide as matrix, in the oxide dispersal oxide matrix of cobalt, cobalt element massfraction in ceramic particle is 1 ~ 20%;
Described oxide is that high temperature sintering can become particulate material, such as, in zirconia, aluminium oxide, titanium dioxide one or more; Described carbonide is that high temperature sintering can become particulate material, such as, in titanium carbide, tantalum carbide, tungsten carbide one or more.
Preferably, the thickness of described low-temperature carbonization silicon layer is 10 ~ 90 μm, and the thickness of internal layer pyrolysis layer of charcoal is 20 ~ 120 μm, and the thickness of high temperature cabonization silicon layer is 20 ~ 90 μm, and the thickness of outer pyrolysis layer of charcoal is 20 ~ 100 μm.The one that described internal layer pyrolysis layer of charcoal and outer pyrolysis layer of charcoal are fine and close pyrolysis layer of charcoal independently of each other, loose pyrolysis layer of charcoal, internal layer loosen in outer fine and close compound pyrolysis layer of charcoal.
Pyrolytic carbon is divided into loose and fine and close pyrolytic carbon because density is different.The density of loose pyrolytic carbon is less than 1.1g/cm
3, the density of fine and close pyrolytic carbon is generally 1.8 ~ 2.0g/cm
3.Function aspects, the swelling of loose pyrolysis layer of charcoal dominant absorption core slug particle and and store the gas that core core produces.The deposition that interior fine and close pyrolytic carbon is SiC provides good interface, and outer fine and close pyrolytic carbon protection particle is from the impact of external environment.Successively can to determine that compound pyrolysis layer of charcoal is that internal layer loosens outer fine and close or contrary for coated order, but according to the actual requirements, the compound pyrolysis layer of charcoal designed in the present invention is internal layer is loose pyrolysis layer of charcoal, the outer structure for fine and close pyrolysis layer of charcoal.
Wherein, described low-temperature carbonization silicon layer is that chlorinated silane is obtained by chemical vapor deposition at 1200 ~ 1450 DEG C; Described high temperature cabonization silicon layer is that chlorinated silane is obtained by chemical vapor deposition at 1550 ~ 1650 DEG C.Low temperature SiC is different from High Temperature SiC, and here for preventing the spilling of coated process cobalt, innermost layer SiC temperature of plate is lower.
Chlorinated silane refers to methyl trichlorosilane, dimethyldichlorosilane or tri-methyl-chlorosilane.
The preparation method containing cobalt coated particle that the present invention proposes, comprises step:
1) fluidized-bed reactor is heated to 1000 ~ 1200 DEG C under an argon atmosphere, puts into the ceramic particle containing cobalt;
2) fluidized-bed reactor is heated to 1200 ~ 1450 DEG C, with the one in methyl trichlorosilane, dimethyldichlorosilane or tri-methyl-chlorosilane for precursor material, be heated to be steam, precursor material steam take hydrogen as carrier band gas, be passed in fluidized-bed reactor, carry out chemical vapor deposition and obtain low-temperature carbonization silicon layer, the time that chemical vapor deposition is carried out is 1 ~ 6h;
3) fluidized-bed reaction actuator temperature is controlled to be 1100 ~ 1400 DEG C, pass into acetylene or propylene gas carries out the coated of internal layer pyrolysis layer of charcoal;
4) fluidized-bed reaction actuator temperature is risen to 1500 ~ 1650 DEG C, precursor material steam is that carrier band gas is passed in fluidized-bed reactor with hydrogen, and carry out chemical vapor deposition and obtain high temperature cabonization silicon layer, the time that chemical vapor deposition is carried out is 1 ~ 4h;
5) temperature of fluidized-bed reactor is controlled at 1100 ~ 1400 DEG C, pass into acetylene or propylene gas carries out the coated of outer pyrolysis layer of charcoal.
Wherein, described step 2) in precursor material at 25 ~ 60 DEG C, be heated to be steam; Fluidizing gas is argon gas and/or hydrogen, and hydrogen is the carrier band gas of precursor vapor, and the throughput ratio of carrier band gas and fluidizing gas is 0.01 ~ 0.2.
Described precursor material steam can adopt the mode of electrical heating or water bath with thermostatic control to produce,
Wherein, described internal layer pyrolysis layer of charcoal and outer pyrolysis layer of charcoal are one that fine and close pyrolysis layer of charcoal, loose pyrolysis layer of charcoal, internal layer loosen in outer fine and close compound pyrolysis layer of charcoal independently of each other;
Wherein, loose pyrolysis layer of charcoal temperature of plate is 1100 ~ 1250 DEG C, and the coated time is 20 ~ 400s, and fluidizing gas is argon gas, and reacting gas is acetylene, and the volume flow ratio of fluidizing gas and reacting gas is 0.2 ~ 4.0;
Fine and close pyrolysis layer of charcoal temperature of plate is 1300 ~ 1400 DEG C, and the coated time is 40 ~ 600s fluidizing gas is argon gas, and reacting gas is propylene, and the volume flow ratio of fluidizing gas and reacting gas is 0.2 ~ 4.0; First coated loose pyrolysis layer of charcoal coated fine and close pyrolysis layer of charcoal again, then internal layer loosens outer fine and close compound pyrolysis layer of charcoal.
Wherein, described step 4) middle employing Ar and H
2for fluidizing gas, the volume flow ratio scope Ar/H of two kinds of gases
2be 0 ~ 0.9.The volume flow ratio scope of carrier band gas and fluidizing gas is 0.01 ~ 0.2.
Further, described step 5) after coated end, with stove cooling under grain fluidized state, be cooled to after room temperature from bottom discharge.
The application containing cobalt coated particle that the present invention proposes, is specially, and is put in nuclear fuel element, carries out spike and the identification of fuel element in reactor by described containing cobalt coated particle.
Beneficial effect of the present invention is:
The present invention proposes a kind of multilayer coating structure of full pottery containing cobalt coated particle form, cobalt element is strapped in the inside of coated particle.Especially, the present invention devises the innermost layer of a kind of low-temperature carbonization silicon layer as clad, prevents the precipitation of cobalt in coated process and subsequent treatment, and under avoiding the interior service condition of heap, tracer grain is on the impact of reactor internal environment.
Present invention process flow process is simple, and technological operation is convenient, and cost is low, can realize multilayer coating structure continuously, be conducive to realizing industrialized mass in vertical fluidized bed.
Accompanying drawing explanation
Fig. 1 is that the present invention contains cobalt coated particle design diagram;
Fig. 2 is the stereoscan photograph of the embodiment of the present invention 1 gained containing cobalt granule;
Fig. 3 is that the embodiment of the present invention 1 gained is containing the scanning of cobalt granule cross sectional elements distributing line;
Fig. 4 is that the embodiment of the present invention 1 gained is containing cobalt granule cross sectional elements distribution Surface scan.
Embodiment
Now with following examples, the present invention is described, but is not used for limiting the scope of the invention.The means used in embodiment, if no special instructions, all use the means of this area routine.
The tracer grain form of the present invention's design as shown in Figure 1.Be designed to internal layer low temperature SiC layer from inside to outside respectively, internal layer pyrolysis layer of charcoal, outer High Temperature SiC layer, outer pyrolysis layer of charcoal.Wherein pyrolysis layer of charcoal can comprise loose pyrolytic carbon and fine and close pyrolytic carbon, and the form of pyrolytic carbon can be individual layer also can be two-layer or multilayer.
Embodiment 1:
Fluidized-bed reactor is heated to 1100 DEG C under an argon atmosphere; Adopt Ar and H
2mixed gas be fluidizing gas, H
2flow be the flow of 6L/min, Ar be 1.0L/min, 40g ZrO
2put into fluidized bed when-CoO (based on particle gross mass, the massfraction of CoO is 3%) particle is 1100 DEG C in fluidized bed reaction zone and carry out fluidisation, average diameter of particles is 600 μm.
The steam of methyl trichlorosilane, constant temperature is at 35 DEG C, and fluidized bed reaction zone is persistently overheating passes into methyl trichlorosilane steam, H to when 1430 DEG C
2for carrier band gas, carrier band airshed is 0.6L/min, and the reaction time is 2h, obtains low-temperature carbonization silicon layer.Be cooled to 1150 DEG C, the flow regulating Ar is 4.0L/min, and acetylene flow is 5L/min, and the reaction time is that 40s obtains loose pyrolysis layer of charcoal.Fluidized bed reaction zone is warming up to 1350 DEG C, and the flow regulating Ar is 4.0L/min, and propylene flow is 2.5L/min, and the reaction time is that 160s obtains fine and close pyrolysis layer of charcoal, and loose pyrolysis layer of charcoal and fine and close pyrolysis layer of charcoal compound form internal layer pyrolysis layer of charcoal.
Regulate the gas flow entering fluidized bed reaction zone, H
2flow be the flow of 6L/min, Ar be 1.0L/min, be warming up to 1580 DEG C and pass into methyl trichlorosilane steam, H
2for carrier band gas, carrier band airshed is 0.6L/min, and the reaction time is 2h, obtains high temperature cabonization silicon layer.The temperature of fluidized bed reaction zone is down to 1350 DEG C, and the flow regulating Ar is 4.0L/min, and propylene flow is 2.5L/min, and the reaction time is that 160s obtains outer fine and close pyrolysis layer of charcoal.After coated end, with stove cooling under grain fluidized state, be cooled to after room temperature from bottom discharge.
Obtain the stereoscan photograph of particle after edge sample grinding and polishing (Fig. 2 a amplifies 40 times, Fig. 2 b amplifies 270 times) as shown in Figure 2 after coated, multilayer coating structure can be seen clearly.Internal layer is the core core of ceramic matrix, core core is of a size of 600 μm, from core core outwards successively coated low-temperature carbonization silicon layer (thickness 30-40 μm) internal layer to loosen pyrolysis layer of charcoal (thickness 40-50 μm), pyrolysis layer of charcoal (thickness 40-50 μm), high temperature cabonization silicon layer (thickness is 30 ~ 40 μm) and outer pyrolysis layer of charcoal (thickness 40-50 μm).
The element line distribution of each layer and EDS maps as shown in Figure 3, Figure 4, can be found out that cobalt element is only present in core core, not detect in each clad, illustrate that cobalt element has been bound in the inside of core core, outwards do not spread.
Embodiment 2
Fluidized-bed reactor is heated to 1100 DEG C under an argon atmosphere; Adopt Ar and H
2mixed gas be fluidizing gas, H
2flow be the flow of 8L/min, Ar be 0.6L/min, 40gZrO
2-CoO (based on particle gross mass, the massfraction of CoO is 6%) particle is put into fluidized bed and is carried out fluidisation 1100 DEG C time, and average diameter of particles is 800 μm.
Methyl trichlorosilane water bath with thermostatic control is made as the steam of 35 DEG C, and fluidized bed is persistently overheating passes into methyl trichlorosilane steam, H to 1430 DEG C
2for carrier band gas, carrier band airshed is 0.6L/min, and the reaction time is 3h, obtains low-temperature carbonization silicon layer.Fluidized bed is cooled to 1150 DEG C, and the flow regulating Ar is 4.0L/min, and acetylene flow is 5L/min, and the reaction time is that 40s obtains loose pyrolysis layer of charcoal.Regulate the gas flow entering fluidized bed reaction zone, H
2flow be the flow of 8L/min, Ar be 0.6L/min, be warming up to 1600 DEG C and pass into methyl trichlorosilane steam, H
2for carrier band gas, carrier band airshed is 0.6L/min, and the reaction time is 2h, obtains high temperature cabonization silicon layer.Be cooled to 1400 DEG C, the flow regulating Ar is 4.0L/min, and propylene flow is 3.5L/min, and the reaction time is that 200s obtains outer fine and close pyrolysis layer of charcoal.After coated end, with stove cooling under grain fluidized state, be cooled to after room temperature from bottom discharge.
Obtain particle after coated to cut open, multilayer coating structure can be seen clearly.Internal layer is the core core of ceramic matrix, core core is of a size of 800 μm, from core core outwards successively coated low-temperature carbonization silicon layer (thickness 50-60 μm) internal layer to loosen pyrolysis layer of charcoal (thickness 50-60 μm), high temperature cabonization silicon layer (thickness is 40 ~ 50 μm) and outer pyrolysis layer of charcoal (thickness 50-60 μm).
Embodiment 3
Fluidized-bed reactor is heated to 1100 DEG C under an argon atmosphere; Adopt Ar and H
2mixed gas be fluidizing gas, H
2flow be the flow of 6L/min, Ar be 1.0L/min, 40g ZrO
2-CoO (based on particle gross mass, the massfraction of CoO is 8%) particle is put into fluidized bed and is carried out fluidisation 1100 DEG C time, and average diameter of particles is 600 μm.
Dimethyldichlorosilane steam at 30 DEG C, persistently overheating passes into dimethyldichlorosilane steam, H to 1380 DEG C with water bath with thermostatic control constant temperature
2for carrier band gas, carrier band airshed is 0.4L/min, and the reaction time is 2h, obtains low-temperature carbonization silicon layer.Fluidized bed reaction zone is warming up to 1350 DEG C, and the flow regulating Ar is 4.0L/min, and propylene flow is 2.0L/min, and the reaction time is that 160s obtains interior fine and close pyrolysis layer of charcoal.Adjusting gas flow, H
2flow be the flow of 6L/min, Ar be 1.0L/min, be warming up to 1550 DEG C and pass into dimethyldichlorosilane steam, H
2for carrier band gas, carrier band airshed is 0.6L/min, and the reaction time is 2h, obtains high temperature cabonization silicon layer.Be cooled to 1350 DEG C, the flow regulating Ar is 4.0L/min, and propylene flow is 2.0L/min, and the reaction time is that 160s obtains outer fine and close pyrolysis layer of charcoal.After coated end, with stove cooling under grain fluidized state, be cooled to after room temperature from bottom discharge.
Obtain particle after coated to cut open, multilayer coating structure can be seen clearly.Internal layer is the core core of ceramic matrix, core core is of a size of 600 μm, from outwards coated low-temperature carbonization silicon layer (thickness 30-40 μm) inner compact layer pyrolysis layer of charcoal (thickness 30-40 μm) successively of core core, high temperature cabonization silicon layer (thickness is 40 ~ 50 μm) and outer pyrolysis layer of charcoal (thickness 30-40 μm).
Embodiment 4
Fluidized-bed reactor is heated to 1100 DEG C under an argon atmosphere; Adopt Ar and H
2mixed gas be fluidizing gas, H
2flow be the flow of 2L/min, Ar be 3.0L/min, 40g ZrO
2-CoO (based on particle gross mass, the massfraction of CoO is 6%) particle is put into fluidized bed and is carried out fluidisation 1100 DEG C time, and average diameter of particles is 700 μm.
Methyl trichlorosilane steam at 35 DEG C, persistently overheating passes into methyl trichlorosilane steam, H to 1450 DEG C with water bath with thermostatic control constant temperature
2for carrier band gas, carrier band airshed is 0.5L/min, and the reaction time is 5h, obtains low-temperature carbonization silicon layer.The reaction zone of fluidized bed is cooled to 1400 DEG C, and the flow regulating Ar is 3.0L/min, and propylene flow is 5.0L/min, and the reaction time is that 260s obtains interior fine and close pyrolysis layer of charcoal.Adjusting gas flow, H
2flow be the flow of 2L/min, Ar be 2.0L/min, be warming up to 1580 DEG C and pass into methyl trichlorosilane steam, H
2for carrier band gas, carrier band airshed is 0.6L/min, and the reaction time is 3h, obtains high temperature cabonization silicon layer.Be cooled to 1400 DEG C, the flow regulating Ar is 3.0L/min, and propylene flow is 5.0L/min, and the reaction time is that 260s obtains outer fine and close pyrolysis layer of charcoal.After coated end, with stove cooling under grain fluidized state, be cooled to after room temperature from bottom discharge.
Obtain particle after coated to cut open, multilayer coating structure can be seen clearly.Internal layer is the core core of ceramic matrix, core core is of a size of 700 μm, from fine and close pyrolysis layer of charcoal (thickness 60-70 μm) of outwards coated low-temperature carbonization silicon layer (thickness 70-80 μm) inner compact layer pyrolysis layer of charcoal (thickness 60-70 μm) successively of core core, high temperature cabonization silicon layer (thickness is 60 ~ 70 μm) and skin.
Embodiment 5
Fluidized-bed reactor is heated to 1050 DEG C under an argon atmosphere; Adopt Ar and H
2mixed gas be fluidizing gas, H
2flow be the flow of 18L/min, Ar be that 2.0L/min, 60g WC-Co (based on particle gross mass, the massfraction of CoO is 6%) particle is put into fluidized bed and carried out fluidisation 1050 DEG C time, average diameter of particles is 600 μm.Methyl trichlorosilane constant temperature, at 35 DEG C, persistently overheatingly passes into methyl trichlorosilane, H to 1400 DEG C
2for carrier band gas, carrier band airshed is 0.6L/min, and the reaction time is 2h, obtains low-temperature carbonization silicon layer.Be cooled to 1350 DEG C, the flow regulating Ar is 6.0L/min, and propylene flow is 4.5L/min, and the reaction time is that 160s obtains interior fine and close pyrolysis layer of charcoal.Adjusting gas flow, H
2flow be the flow of 18L/min, Ar be 2.0L/min, be warming up to 1580 DEG C and pass into methyl trichlorosilane, H
2for carrier band gas, carrier band airshed is 0.6L/min, and the reaction time is 2h, obtains high temperature cabonization silicon layer.Be cooled to 1350 DEG C, the flow regulating Ar is 6.0L/min, and propylene flow is 4L/min, and the reaction time is that 160s obtains outer fine and close pyrolysis layer of charcoal.
Obtain particle after coated to cut open, multilayer coating structure can be seen clearly.Internal layer is the core core of ceramic matrix, core core is of a size of 600 μm, from fine and close pyrolysis layer of charcoal (thickness 40-50 μm) of outwards coated low-temperature carbonization silicon layer (thickness 40-50 μm) inner compact layer pyrolysis layer of charcoal (thickness 40-50 μm) successively of core core, high temperature cabonization silicon layer (thickness is 40 ~ 50 μm) and skin.
Above embodiment is only be described the preferred embodiment of the present invention; not scope of the present invention is limited; under not departing from the present invention and designing the prerequisite of spirit; the various modification that the common engineering technical personnel in this area make technical scheme of the present invention and improvement, all should fall in protection domain that claims of the present invention determine.
Claims (9)
1. one kind contains cobalt coated particle, it is characterized in that, described have sandwich construction containing cobalt coated particle, and the core core of particle is the ceramic particle containing cobalt, described ceramic particle is that the oxide of cobalt or cobalt is dispersed in carbonide or oxide matrix with carbonide or oxide for matrix; Core core is of a size of 200 ~ 900 μm, and core core is 0.1% ~ 35% containing cobalt massfraction; From core the core outside coated silicon carbide layer of low temperature, internal layer pyrolysis layer of charcoal, the coated silicon carbide layer of high temperature and outer pyrolysis layer of charcoal successively.
2. according to claim 1 containing cobalt coated particle, it is characterized in that, described ceramic particle take carbonide as matrix, and in simple substance cobalt dispersed carbides matrix, simple substance cobalt massfraction in ceramic particle is 1% ~ 20%; Or described ceramic particle take oxide as matrix, in the oxide dispersal oxide matrix of cobalt, cobalt element massfraction in ceramic particle is 1% ~ 20%;
Described oxide is one or more in zirconia, aluminium oxide, titanium dioxide; Described carbonide is one or more in titanium carbide, tantalum carbide, tungsten carbide.
3. according to claim 1 containing cobalt coated particle, it is characterized in that, the thickness of described low-temperature carbonization silicon layer is 10 ~ 90 μm, and the thickness of internal layer pyrolysis layer of charcoal is 20 ~ 120 μm, the thickness of high temperature cabonization silicon layer is 20 ~ 90 μm, and the thickness of outer pyrolysis layer of charcoal is 20 ~ 100 μm; The one that described internal layer pyrolysis layer of charcoal and outer pyrolysis layer of charcoal are fine and close pyrolysis layer of charcoal independently of each other, loose pyrolysis layer of charcoal, internal layer loosen in outer fine and close compound pyrolysis layer of charcoal.
4. according to claim 1 containing cobalt coated particle, it is characterized in that, described low-temperature carbonization silicon layer is that chlorinated silane is obtained by fluidized bed-chemical gaseous phase depositing process at 1200 ~ 1450 DEG C; Described high temperature cabonization silicon layer is that chlorinated silane is obtained by fluidized bed-chemical gaseous phase depositing process at 1550 ~ 1650 DEG C.
5. the arbitrary described preparation method containing cobalt coated particle of Claims 1 to 4, is characterized in that, comprise step:
1) fluidized-bed reactor is heated to 1000 ~ 1200 DEG C under an argon atmosphere, puts into the ceramic particle containing cobalt;
2) fluidized-bed reactor is heated to 1200 ~ 1450 DEG C, with the one in methyl trichlorosilane, dimethyldichlorosilane or tri-methyl-chlorosilane for precursor material, be heated to be steam, precursor material steam take hydrogen as carrier band gas, be passed in fluidized-bed reactor, carry out chemical vapor deposition and obtain low-temperature carbonization silicon layer, the time that chemical vapor deposition is carried out is 1 ~ 6h;
3) fluidized-bed reaction actuator temperature is controlled to be 1100 ~ 1400 DEG C, pass into acetylene or propylene gas carries out the coated of internal layer pyrolysis layer of charcoal;
4) fluidized-bed reaction actuator temperature is risen to 1500 ~ 1650 DEG C, precursor material steam is that carrier band gas is passed in fluidized-bed reactor with hydrogen, and carry out chemical vapor deposition and obtain high temperature cabonization silicon layer, the time that chemical vapor deposition is carried out is 1 ~ 4h;
5) temperature of fluidized-bed reactor is controlled at 1100 ~ 1400 DEG C, pass into acetylene or propylene gas carries out the coated of outer pyrolysis layer of charcoal.
6. preparation method according to claim 5, is characterized in that, described step 2) in precursor material at 25 ~ 60 DEG C, be heated to be steam; Fluidizing gas is argon gas and/or hydrogen, and hydrogen is the carrier band gas of precursor vapor, and the volume flow ratio of carrier band gas and fluidizing gas is 0.01 ~ 0.2.
7. preparation method according to claim 5, is characterized in that, the one that described internal layer pyrolysis layer of charcoal and outer pyrolysis layer of charcoal are fine and close pyrolysis layer of charcoal independently of each other, loose pyrolysis layer of charcoal, internal layer loosen in outer fine and close compound pyrolysis layer of charcoal;
Wherein, loose pyrolysis layer of charcoal temperature of plate is 1100 DEG C ~ 1250 DEG C, and the coated time is 20 ~ 400s, and fluidizing gas is argon gas, and reacting gas is acetylene, and the throughput ratio of fluidizing gas and reacting gas is 0.2 ~ 4.0;
Fine and close pyrolysis layer of charcoal temperature of plate is 1300 ~ 1400 DEG C, and the coated time is 40 ~ 600s fluidizing gas is argon gas, and reacting gas is propylene, and the throughput ratio of fluidizing gas and reacting gas is 0.2 ~ 4.0; First coated loose pyrolysis layer of charcoal coated fine and close pyrolysis layer of charcoal again, then internal layer loosens outer fine and close compound pyrolysis layer of charcoal.
8. preparation method according to claim 5, is characterized in that, described step 4) in adopt argon gas and hydrogen to be fluidizing gas, the throughput ratio scope Ar/H of two kinds of gases
2be 0 ~ 0.9; The throughput ratio scope of carrier band gas and fluidizing gas is 0.01 ~ 0.2.
9. the arbitrary described application containing cobalt spike coated particle of Claims 1 to 4, is characterized in that, the described cobalt coated particle that contains is put in fuel element, carries out spike and the identification of nuclear fuel element in reactor.
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| CN108531884A (en) * | 2018-05-25 | 2018-09-14 | 中国科学院过程工程研究所 | A kind of cobalt coating ceramic alloy-based composite hard raw powder's production technology |
| CN108675300A (en) * | 2018-06-15 | 2018-10-19 | 清华大学 | A kind of nuclear shell structure nano composite particles and preparation method thereof, its preparation facilities |
| CN109326363A (en) * | 2018-09-29 | 2019-02-12 | 中广核研究院有限公司 | Diffusion-type fuel pellet and preparation method thereof, fuel rod |
| CN111724919A (en) * | 2020-06-29 | 2020-09-29 | 清华大学 | Coated fuel particle containing burnable poison coating layer, pellet, fuel element and preparation method thereof |
| CN113658724A (en) * | 2021-08-17 | 2021-11-16 | 西北工业大学 | Ceramic composite fuel pellet and preparation method and application thereof |
Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3992258A (en) * | 1974-01-07 | 1976-11-16 | Westinghouse Electric Corporation | Coated nuclear fuel particles and process for making the same |
| US4267019A (en) * | 1978-05-10 | 1981-05-12 | General Atomic Company | Nuclear fuel particles |
| US4597936A (en) * | 1983-10-12 | 1986-07-01 | Ga Technologies Inc. | Lithium-containing neutron target particle |
| US20070263762A1 (en) * | 2004-03-01 | 2007-11-15 | Pebble Bed Modular Reactor (Proprietary) Limited | Nuclear Fuel |
| US20110091004A1 (en) * | 2007-10-04 | 2011-04-21 | Lawrence Livermore National Security, Llc | Triso fuel for high burn-up nuclear engine |
-
2015
- 2015-03-19 CN CN201510122718.2A patent/CN104810065B/en active Active
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3992258A (en) * | 1974-01-07 | 1976-11-16 | Westinghouse Electric Corporation | Coated nuclear fuel particles and process for making the same |
| US4267019A (en) * | 1978-05-10 | 1981-05-12 | General Atomic Company | Nuclear fuel particles |
| US4597936A (en) * | 1983-10-12 | 1986-07-01 | Ga Technologies Inc. | Lithium-containing neutron target particle |
| US20070263762A1 (en) * | 2004-03-01 | 2007-11-15 | Pebble Bed Modular Reactor (Proprietary) Limited | Nuclear Fuel |
| US20110091004A1 (en) * | 2007-10-04 | 2011-04-21 | Lawrence Livermore National Security, Llc | Triso fuel for high burn-up nuclear engine |
Non-Patent Citations (3)
| Title |
|---|
| 刘荣正 等: "HTGR包覆燃料颗粒碳化硅层细晶化研究", 《原子能科学技术》 * |
| 刘裔兴 等: "外凝胶法制备含钴的核壳双层凝胶微球的影响因素", 《第十八届全国高技术陶瓷学术年会》 * |
| 邵友林 等: "包覆燃料颗粒及其应用", 《原子能科学技术》 * |
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| CN108531884A (en) * | 2018-05-25 | 2018-09-14 | 中国科学院过程工程研究所 | A kind of cobalt coating ceramic alloy-based composite hard raw powder's production technology |
| CN108675300A (en) * | 2018-06-15 | 2018-10-19 | 清华大学 | A kind of nuclear shell structure nano composite particles and preparation method thereof, its preparation facilities |
| CN109326363A (en) * | 2018-09-29 | 2019-02-12 | 中广核研究院有限公司 | Diffusion-type fuel pellet and preparation method thereof, fuel rod |
| CN109326363B (en) * | 2018-09-29 | 2020-12-29 | 中广核研究院有限公司 | Dispersed fuel pellet, preparation method thereof and fuel rod |
| CN111724919A (en) * | 2020-06-29 | 2020-09-29 | 清华大学 | Coated fuel particle containing burnable poison coating layer, pellet, fuel element and preparation method thereof |
| CN111724919B (en) * | 2020-06-29 | 2022-09-09 | 清华大学 | Coated fuel particle containing burnable poison coating layer, pellet, fuel element and preparation method thereof |
| CN113658724A (en) * | 2021-08-17 | 2021-11-16 | 西北工业大学 | Ceramic composite fuel pellet and preparation method and application thereof |
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