GB1602821A - Creación de Inventos y Patentes con Inteligencia Artificial

GB1602821A – Ceramic powder material and method for manufacturing the same
– Google Patents

GB1602821A – Ceramic powder material and method for manufacturing the same
– Google Patents
Ceramic powder material and method for manufacturing the same

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Publication number
GB1602821A

GB1602821A
GB1497/78A
GB149778A
GB1602821A
GB 1602821 A
GB1602821 A
GB 1602821A
GB 1497/78 A
GB1497/78 A
GB 1497/78A
GB 149778 A
GB149778 A
GB 149778A
GB 1602821 A
GB1602821 A
GB 1602821A
Authority
GB
United Kingdom
Prior art keywords
weight
ceramic powder
yttrium
silicon nitride
aluminium
Prior art date
1977-01-13
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)

Expired

Application number
GB1497/78A
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)

Toshiba Corp

Original Assignee
Tokyo Shibaura Electric Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
1977-01-13
Filing date
1978-01-13
Publication date
1981-11-18

1977-01-13
Priority claimed from JP52001949A
external-priority
patent/JPS6035315B2/en

1977-09-22
Priority claimed from JP52113235A
external-priority
patent/JPS596836B2/en

1978-01-13
Application filed by Tokyo Shibaura Electric Co Ltd
filed
Critical
Tokyo Shibaura Electric Co Ltd

1978-02-13
Priority to GB3080780A
priority
Critical
patent/GB1602822A/en

1981-11-18
Publication of GB1602821A
publication
Critical
patent/GB1602821A/en

Status
Expired
legal-status
Critical
Current

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Classifications

C—CHEMISTRY; METALLURGY

C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES

C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE

C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products

C04B35/515—Shaped 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

C04B35/58—Shaped 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

C04B35/584—Shaped 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 based on silicon nitride

C04B35/593—Shaped 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 based on silicon nitride obtained by pressure sintering

C—CHEMISTRY; METALLURGY

C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES

C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE

C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products

Description

PATENT SPECIFICATION ( 11) 1602821
-I ( 21) Application No 1497/78 ( 22) Filed 13 Jan 1978 N ( 31) Convention Application No 52/001 9499 ( 32) Filed 13 Jan 1977 O ( 31) Convention Application No 52/113 235 e ( 32) Filed 22 Sept 1977 in -( 33) Japan (JP) ( 44) Complete Specification published 18 Nov 1981 ( 51) INT CL 3 C 04 B 35/58 ( 52) Index at acceptance C 1 J 1 21 33 9 X ( 72) Inventors KATSUTOSHI NISH 1 DA, MICHIYASU KOMATSU and TADASHI MIYANO ( 54) CERAMIC POWDER MATERIAL AND METHOD FOR MANUFACTURING THE SAME ( 71) We, TOKYO SHIBAURA ELECTRIC COMPANY LIMITED, a Japanese corporation, of 72 Horikawa-cho, Saiwai-ku, Kawasaki-shi, Japan, do hereby declare the invention, for which we pray that a patent may be granted to us, and the method by which it is to be performed, to be particularly described in and by the
S following statement: 5
This invention relates to improvements in raw ceramic powder materials adapted to provide a sintered ceramic product of high mechanical strength and more particularly to improvements on raw ceramic powder material mainly consisting of silicon nitride.
Worldwide studies have been made of sintered silicon nitride which displays 10 prominent mechanical strength at high temperature Known processes developed to this end include, for example, that which hot-presses silicon nitride powder mixed with magnesia, and that which similarly hot-presses silicon nitride powder mixed with yttria These processes are found to provide a dense sintered product of silicon nitride However, a more dense construction does not offer excellent mechanical 15 strength at high temperature The reason is that a simply densified sintered product contains glassy material, which gives rise to a decline in the high temperature mechanical strength of the product.
The present inventor has studied the optimum composition of raw ceramic powder material to decrease the content of glassy component, and accomplished this 20 invention.
It is accordingly an object of this invention to provide raw ceramic powder material adapted to manufacture a sintered product having excellent mechanical strength at high temperature.
Another object of this invention is to provide such raw ceramic powder material 25 as enables the content of glassy material in a sintered product to be decreased.
Still another object of the invention is to provide a method for efficiently preparing the above-mentioned raw ceramic powder material.
The fundamental technical concept of this invention is to restrict the content of oxygen in the raw ceramic powder material Silicon nitride powder contains various 3 kinds of impurities, and is not formed of silicon and nitrogen alone For instance, silica is generally deposited on the surface of the particles of silicon nitride powder.
Further, iron and calcium, for example, are often present in the silicon nitride powder as unavoidable impurities Many of these impurities are generally present in raw ceramic powder material in the form combined with oxygen The resultant oxides are 35 supposed to cause a decline in the high temperature mechanical strength of a sintered product.
The present inventor has carried out various experiments and as a result has considered that particularly the amount of oxygen combined with the abovementioned unavoidable impurities raises problems It has been found that a raw ceramic powder 40 material comprising mainly silicon nitride together with aluminium and yttrium less than a maximum amount of oxygen is adapted to provide a sintered product having prominent high temperature mechanical strength.
2 1,602,821 2 According to the invention, therefore, there is provided a ceramic powder material comprising silicon nitride powder containing from 0 05 to 2 5 % by weight of aluminium and from 0 4 to 8 0 % by weight of yttrium, and in which all or a part of the yttrium contained in the silicon nitride powder is present in the form of a crystalline compound of silicon nitride and yttrium oxide and in which the total % 5 by weight Wo of oxygen as measured by activation analysis satisfies the following formula indicating the % by weight W,, of aluminium and the % by weight W, of yttrium:
atomic weight atomic weight of oxygen of oxygen WO X + 15 X (WA 1 X atomic weight atomic weight of aluminium of yttrium and X is smaller than or equal to 2 0 The term X given in the above formula is 10 desired to have a smaller value than 1 0 or most preferably 0 5.
For the preparation of desired raw ceramic powder material from silicon nitride powder mixed with alumina and yttria, it is advised to heat raw silicon nitride powder containing 0 1 to 5 % by weight of alumina and 0 5 to 10 % by weight of yttria to a temperature ranging between 1,400 ‘C and 1,900 ‘C, preferably between 1, 500 ‘C and 15 1,850 ‘C, or more preferably between 1,550 ‘C and 1,800 ‘C.
A part or the whole of yttrium be present in the heated mass is in the form of a crystalline compound consisting of silicon nitride and yttrium oxide The presence of this crystalline compound can be ascertained by the X-ray diffraction analysis For the growth of said crystalline compound, it is advised to apply heating at a higher 20 temperature than 1,600 ‘C.
The raw ceramic powder material can be heated in a far shorter time than in the prior art, if said heating is carried out (as described in our copending application
No 80 30807 (Serial No 1 602 822)) in the presence of a nonsintered molding of ceramic material or a sintered molding of ceramic material having a porosity of at 25 least 10 % The ceramic material molded in the sintered or nonsintered form includes aluminium nitride, boron nitride, titanium nitride, silicon nitride and aluminium oxide Among the above-listed compounds, aluminium nitride displays the most prominent effect of shortening heating time.
Application of the above-mentioned nonsintered or sintered ceramic molding 30 causes oxygen-containing gas evolved from heated raw ceramic powder material re be securely absorbed in said molding or to be given off to the outside therethrough, thereby supposedly carrying out effective deoxidation.
It is preferred that the above-mentioned heating be undertaken by charging the raw ceramic powder material and the aforesaid molding in a vessel made of such material as is nonreactive with the charged mass The desired vessel is made of aluminium nitride Heating is carried out in a nonoxidizing atmosphere such as nitrogen gas or any other inert gas.
The nonsintered ceramic molding acting as a heating time reducer is prepared by 40 mixing said material with an organic binder, followed by molding The nonsintered ceramic molding acting as a heating time reducer generally has a porosity ranging approximately between 35 and 55 % For the object of this invention, however the nonsintered molding can be produced with a porosity falling outside of the abovementioned range A sintered ceramic molding acting as a heating time reducer having 45 a porosity of at least 10 % can be prepared by heating said nonsintered molding at a high temperature in a nonoxidizing atmosphere.
Table 1 below shows the examples of the methods of manufacturing a heating time reducer from nonsintered and sintered moldings of aluminium nitride with various degrees of porosity.
1,602,821 TABLE 1
Form of heating Porosity time reducer (N) Manufacturing method Nonsintered 70 Commercially available aluminium nitride powder is pulverized in a ball mill, An organic binder is added to the pulverized mass, followed by molding at a pressure of 50 to 100 Kg/cm 2 ‘ Substantially the same process as described above is used, except that the pressure applied ranges between 500 and 700 Kg /cm’.
Coarse aluminium nitride particles and fine aluminium nitride particles are mixed in the ratio of 7: 3, An organic binder is added to the mixture, followed by molding at a pressure of 5,000 Kg/cm 2 Sintered 50 The above-mentioned nonsintered aluminium nitride having a porosity of 70 % is sintered one hour at 1,700 ‘C in an atmosphere of nitrogen.
The above-mentioned nonsintered aluminium nitride having a porosity of 50 % is sintered two hours at 1,8001 C in an atmosphere of nitrogen, 0 5 % by weight of yttria is added to fine aluminium nitride powder, After molded, the mass is sintered two hours at 1,8001 C in an atmosphere of nitrogen8 2 % by weight of yttria is added to fine aluminium nitride powder, After molding, the mass is sintered two hours at 1,750 ‘C in an atmosphere of nitrogen.
The nonsintered or sintered molding acting as a heating time reducer used in this invention need not be formed of a single compound, but may be prepared in the form mixed with, for example, yttria, alumina or silica However, it is preferred that these ingredients be added in a smaller amount than 20 % by weight The reason is rhat where the heating time reducer contains a large amount (more than 20 %) of the additives, then undesirable reactions will occur between said additives and the raw ceramic powder.
This invention will be more fully understood by reference to the examples which follow.
In the Examples the raw silicon nitride powders having the elementary analysis given below were employed as starting materials.
Elementary analysis (% by weight) Silicon Nitride Powder Silicon Nitrogen Aluminium Iron Calcium Oxygen A 58 6 36 1 0 25 0 21 4 3 B 57 8 355 0 23 0 35 0 11 3 51 Silicon nitride of the CP-85 grade manufactured by Advanced Materials Engineering Limited, England.
(The oxygen content was determined by activation analysis, the nitrogen content by a gas analyzer, and the content of the other elements by customary wet analytid methods These methods were used to analyze the products of the examples).
EXAMPLE 1 5
Silicon nitride powder A was mixed with alumina and yttria to give a mixture containing 2 5 % by weight of alumina and 4 8 % by weight of yttria The mass was placed in a vessel made of aluminium nitride, followed by heating of 2 hours at 1,750 ‘C On analysis it was found that the heated mass was formed of 55 7 % by weight of silicon, 1 3 % by weight of aluminium 3 8 % by weight of yttrium, 0 31 % 10 by weight of iron, 0 26 % by weight of calcium, 32 6 % by weight of nitrogen and 2.6 % by weight of oxygen As analyzed by X-ray diffraction, a crystalline compound of silicon nitride and yttria (Si N 4 YO,) having a molar ratio of 1: 1 was grown in the heated mass It was found that 90 % of the yttrium content in the raw ceramic powder was present in the form of said silicon yttrium oxynitride crystal compound 15 After moulding, the heated raw ceramic powder was sintered for 2 hours at 1,800 ‘C at a pressure of 500 Kg/cm 2 and the product has a flexural strength of 92 Kg/mm 2 at 1,200 GC.
The flexural strength test was carried out by the three-point bending method under the following conditions: 20 Sample size 3 X 3 X 35 mm Span 20 mm Crosshead speed 0 5 mm/min EXAMPLE 2.
Silicon nitride powder B was used as a starting material X-ray diffraction analysis showed said starting material to contain 87 % of a-type silicon nitride, whose 25 particle size was determined to be 1 8 microns by the Fisher Sub-Sieve Sizer.
% by weight of YO, was added to the raw silicon nitride powder B followed by crushing and mixing for 100 hours in an alumina pot filled with alumina balls The abraded portions of the alumina pot and alumina balls were carried into the crushed silicon nitride powder now mixed with Y 20,, with a resultant increase in the alumina 30 content The crushed silicon nitride powder had a particle size of 1 1 microns as measured by the Fisher Sub-Sieve Sizer, and was analyzed to contain the following elements:
Element Silicon Nitrogen Aluminium Iron Calcium Yttrium Oxygen % by weight 565 347 131 032 0 10 369 5 31 1,602,821 The above-mentioned raw mixed ceramic powder was charged in an aluminium nitride vessel, followed by heating for 2 hours at 1,730 C The heated mass was analyzed by X-ray diffraction to contain a silicon yttrium oxynitride crystal compound (Si N 4 Y 200) A calibration curve showed that 80 % of the Y,,: added to the raw silicon nitride powder was present in the form of said Si:N 4 Y 20: compound The 5 heated raw mixed ceramic powder was analyzed to contain the following elements:
Element Silicon Nitrogen Aluminium Iron Calcium Yttrium Oxygen % by weight 56 6 35 1 1 26 0 30 0 09 3 o 71 2 65 The heated raw powder was sintered 2 hours by the customary hot press process at a temperature of 1,800 C and a pressure of 400 Kg/cm 2 Samples were cut out of the sintered mass The same flexural strength test as applied in Example 1 showed the 10 samples to have a flexural strength of 85 Kg/mm 2 at 1,200 C, that is, a prominent heat resistance.

Claims (4)

WHAT WE CLAIM IS:-

1 A ceramic powder material comprising silicon nitride powder containing from s 15 0 05 to

2 5 % by weight of aluminium and from 0 4 to 8 0 % by weight of yttrium, 15 in which all or a part of the yttrium contained in the silicon nitride powder is present in the form of a crystalline compound of silicon nitride and yttrium oxide and in which the total oxygen content Wo (% by weight) as measured by activation analysis falls within the range expressed by the following formula denoting the relationship between the content of aluminium Wa, (% by weight) and the content oi 20 yttrium Wy (% by weight):
atomic weight atomic weight of oxygen of oxygen atomic weight atomic weight of aluminium of yttrium 2 A ceramic powder according to claim 1, wherein the crystalline compound is a silicon yttrium oxynitride crystal compound (Si N 4 Y 20,).

3 A method of manufacturing a ceramic powder material as claimed in claim 1 25 which comprises heating a raw mixed ceramic powder containing 0 1 to 5 % by weight of alumina, 0 5 to 10 % by weight of yttria and a balance of silicon nitride to a temperature ranging between 1,400 C and 1,900 C.

4 A ceramic powder material as claimed in claim 1 substantially as hereinbefore described with reference to the Examples 30 A method of manufacturing a ceramic powder material, as claimed in claim 3 substantially as hereinbefore described with reference to the Examples.
MARKS & CLERK, Chartered Patent Agents, 57-60 Lincoln’s Inn Fields, London, WC 2 A 3 LS.
Agents for the Applicants.
Printed for Her Majesty’s Stationery Office by the Courier Press, Leamington Spa, 1981.
Published by the Patent Office, 25 Southampton Buildings, London, WC 2 A l AY, from which copies may be obtained.
1,602,821 c

GB1497/78A
1977-01-13
1978-01-13
Ceramic powder material and method for manufacturing the same

Expired

GB1602821A
(en)

Priority Applications (1)

Application Number
Priority Date
Filing Date
Title

GB3080780A

GB1602822A
(en)

1977-09-22
1978-02-13
Method for manufacturing ceramic powder materials

Applications Claiming Priority (2)

Application Number
Priority Date
Filing Date
Title

JP52001949A

JPS6035315B2
(en)

1977-01-13
1977-01-13

Manufacturing method of ceramic powder material

JP52113235A

JPS596836B2
(en)

1977-09-22
1977-09-22

Manufacturing method of ceramic powder material

Publications (1)

Publication Number
Publication Date

GB1602821A
true

GB1602821A
(en)

1981-11-18

Family
ID=26335248
Family Applications (1)

Application Number
Title
Priority Date
Filing Date

GB1497/78A
Expired

GB1602821A
(en)

1977-01-13
1978-01-13
Ceramic powder material and method for manufacturing the same

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US
(1)

US4284432A
(en)

DE
(1)

DE2801474C2
(en)

GB
(1)

GB1602821A
(en)

SE
(2)

SE427650B
(en)

Cited By (1)

* Cited by examiner, † Cited by third party

Publication number
Priority date
Publication date
Assignee
Title

FR2517665A1
(en)

1981-12-08
1983-06-10
Ceraver

PROCESS FOR PRODUCING SILICON NITRIDE FRITTE MATERIAL AND MATERIAL OBTAINED THEREBY

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* Cited by examiner, † Cited by third party

Publication number
Priority date
Publication date
Assignee
Title

DE3162375D1
(en)

1980-08-06
1984-03-29
Feldmuehle Ag
Dense silicon-nitride shaped body containing yttrium oxide, and process for its production

US4511525A
(en)

1981-11-26
1985-04-16
Tokyo Shibaura Denki Kabushiki Kaisha
Process for producing sintered silicon nitride-base body

US5324694A
(en)

1985-06-26
1994-06-28
The Babcock & Wilcox Company
Silicon nitride/boron nitride composite with enhanced fracture toughness

CA1268488A
(en)

1986-10-28
1990-05-01
Russell L. Yeckley
Silicon nitride with improved high temperature strength

JP2577899B2
(en)

1987-01-28
1997-02-05
本田技研工業株式会社

Silicon nitride sintered body and method for producing the same

DE3829503A1
(en)

1988-08-31
1990-03-01
Bayer Ag

SILICON NITRIDE POWDER WITH LOW OXYGEN CONTENT

DE3829504A1
(en)

1988-08-31
1990-03-01
Bayer Ag

SILICON NITRIDE POWDER WITH IMPROVED SURFACE PROPERTIES AND METHOD FOR THE PRODUCTION THEREOF

DE3829502A1
(en)

1988-08-31
1990-03-01
Bayer Ag

SILICON NITRIDE POWDER WITH LOW ISOELECTRIC POINT AND METHOD FOR THE PRODUCTION THEREOF

ES2020104A6
(en)

1990-01-23
1991-07-16
Ercros Sa
Composite ceramic materials for applications in engineering at high temperature and under severe conditions of thermal shock and a process for their production.

US5538675A
(en)

1994-04-14
1996-07-23
The Dow Chemical Company
Method for producing silicon nitride/silicon carbide composite

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Publication date
Assignee
Title

GB970639A
(en)

1960-03-24
1964-09-23
Plessey Co Ltd
Method of producing high density silicon nitride

US3835211A
(en)

1968-12-11
1974-09-10
Lucas Industries Ltd
Silicon nitride products

JPS4921091B1
(en)

1970-08-10
1974-05-29

US3836374A
(en)

1972-01-20
1974-09-17
Norton Co
Hot pressed silicon nitride

US3992497A
(en)

1973-05-18
1976-11-16
Westinghouse Electric Corporation
Pressureless sintering silicon nitride powders

US3830652A
(en)

1973-06-28
1974-08-20
Us Army
Hot pressed, high strength silicon nitride

US4046580A
(en)

1974-06-28
1977-09-06
Tokyo Shibaura Electric Co., Ltd.
Silicon nitride-based sintered material and method for manufacturing the same

US4071371A
(en)

1975-03-06
1978-01-31
Ford Motor Company
High temperature ceramic material suitable for gas turbine applications and a process for producing same

1978

1978-01-12
SE
SE7800350A
patent/SE427650B/en
not_active
IP Right Cessation

1978-01-13
GB
GB1497/78A
patent/GB1602821A/en
not_active
Expired

1978-01-13
DE
DE2801474A
patent/DE2801474C2/en
not_active
Expired

1979

1979-09-21
US
US06/078,584
patent/US4284432A/en
not_active
Expired – Lifetime

1982

1982-12-13
SE
SE8207111A
patent/SE8207111L/en
not_active
Application Discontinuation

Cited By (2)

* Cited by examiner, † Cited by third party

Publication number
Priority date
Publication date
Assignee
Title

FR2517665A1
(en)

1981-12-08
1983-06-10
Ceraver

PROCESS FOR PRODUCING SILICON NITRIDE FRITTE MATERIAL AND MATERIAL OBTAINED THEREBY

EP0081195A1
(en)

1981-12-08
1983-06-15
Ceramiques Et Composites
Method of manufacturing a silicon nitride-based sintered material, and material obtained by this method

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Publication number
Publication date

SE427650B
(en)

1983-04-25

SE8207111D0
(en)

1982-12-13

DE2801474C2
(en)

1985-01-10

US4284432A
(en)

1981-08-18

DE2801474A1
(en)

1978-07-27

SE8207111L
(en)

1982-12-13

SE7800350L
(en)

1978-07-14

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