公开(公告)号：US4687655A

公开(公告)日：1987-08-18

申请号：US850748

申请日：1986-04-11

申请人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth ,  Peter Arnold ,  Johannes Napholcz

发明人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth ,  Peter Arnold ,  Johannes Napholcz

IPC分类号： C04B35/58 ,  C04B35/584 ,  C04B35/591 ,  C04B35/593

CPC分类号： C04B35/591 ,  C04B35/5935 ,  C04B2235/3205 ,  C04B2235/3206 ,  C04B2235/3217 ,  C04B2235/3225 ,  C04B2235/3272 ,  C04B2235/3873 ,  C04B2235/3895 ,  C04B2235/428 ,  C04B2235/5436 ,  C04B2235/5445 ,  C04B2235/6562 ,  C04B2235/6567 ,  C04B2235/661 ,  C04B2235/72 ,  C04B2235/728 ,  C04B2235/77

摘要： The invention is a process for the manufacture of shaped articles of reaction-bonded silicon nitride in which pre-shaped articles of silicon powder are heated in a first stage under a nitrogen gas pressure of at least 6 MPa at a heating rate of not more than 50.degree. C. per hour to a reaction temperature below the melting point of silicon, the article is maintained at the reaction temperature for at least 0.5 hours and subsequently, in a second stage, heating the article at a heating rate of at least 500.degree. C. per hour to a temperature above the melting point of silicon and maintaining the article at that temperature for from 1 to 7 hours. The process can nitridate both pre-shaped articles consisting of silicon powder and, optionally, up to 15% by weight Si.sub.3 N.sub.4 powder and those containing up to 10% by weight of a sintering aid such as Y.sub.2 O.sub.3. In the former case, porous shaped articles having a density of from 87 to 91% TD and, in the latter case, dense shaped articles having a density of more than 98% TD, are obtained. In all cases, in a total nitridation time of less than 15 hours, a conversion of at least 95% of the silicon originally present into silicon nitride is achieved, which, in the finished shaped article, is substantially in the .beta.-modification.

摘要翻译： 本发明是一种反应粘合氮化硅成型制品的制造方法，其中在第一阶段在至少6MPa的氮气压力下加热预成型制品，其加热速率不大于 50℃/小时至低于硅熔点的反应温度，将制品保持在反应温度至少0.5小时，随后在第二阶段以至少500℃的加热速率加热制品 每小时至高于硅熔点的温度，并将制品在该温度下保持1至7小时。 该方法可以将由硅粉末和任选地至多15重量％的Si 3 N 4粉末组成的预成型制品和包含至多10重量％的烧结助剂例如Y 2 O 3的预成型制品进行氮化。 在前一种情况下，得到密度为87〜91％TD的多孔成形制品，在后一种情况下，得到密度大于98％TD的致密成形制品。 在所有情况下，在小于15小时的总氮化时间中，实现了最初存在于氮化硅中的硅的至少95％的转化率，其在成品成型制品中基本上处于β-改性。

公开(公告)号：US4351858A

公开(公告)日：1982-09-28

申请号：US238106

申请日：1981-02-25

申请人： Klaus Hunold ,  Klaus Reinmuth ,  Alfred Lipp ,  Johannes Napholcz ,  Peter Arnold

发明人： Klaus Hunold ,  Klaus Reinmuth ,  Alfred Lipp ,  Johannes Napholcz ,  Peter Arnold

IPC分类号： B22F3/14 ,  B22F3/12 ,  B22F3/15 ,  C04B35/645 ,  B05D3/02

CPC分类号： C04B35/6455 ,  B22F3/1241 ,  B22F3/1266 ,  B22F2998/00

摘要： The invention is a process for the manufacture of substantially pore-free shaped articles from polycrystalline material, such as tungsten carbide, silicon nitride, titanium boride or silicon carbide, in which encased articles preformed from pulverulent materials and having open pores are isostatically hot-pressed in a vacuum-sealed casing of vitreous or ceramic-like material in a high-pressure autoclave using an inert gas as pressure-transfer medium. Before the application of the casing material, a first layer comprising material that can be decomposed or melted, such as an organic wax or a resin-like product, or of a compressible heat-resistant material such as inorganic fibers or felts, is applied to the preformed articles. Then, the encased articles are thermally treated until the glass or ceramic layer is fused or sintered gas-tight. The articles pretreated in this manner are then isostatically hot-pressed.

摘要翻译： 本发明是一种用于从多晶材料制造基本上无孔的成形制品的方法，例如碳化钨，氮化硅，硼化钛或碳化硅，其中由粉状材料预成型并具有开孔的包封制品经均压热压 在使用惰性气体作为压力传递介质的高压高压釜中的玻璃质或陶瓷状材料的真空密封外壳中。 在施加外壳材料之前，将包含可分解或熔化的材料（例如有机蜡或树脂状产品）的第一层或诸如无机纤维或毡的可压缩耐热材料施加到 预成型制品。 然后，将包裹的物品进行热处理，直到玻璃或陶瓷层熔融或烧结为气密。 然后以这种方式预处理的制品被等压热压。

公开(公告)号：US4732620A

公开(公告)日：1988-03-22

申请号：US840989

申请日：1986-03-14

申请人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth ,  Peter Arnold

发明人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth ,  Peter Arnold

IPC分类号： G01K7/02 ,  G01K7/06 ,  H01L35/22 ,  H01L35/32 ,  H01L35/28

CPC分类号： G01K7/06

摘要： The invention is an improved theroelement which comprises a graphite/boron carbide thermocouple, the arms of which are constructed as a tube and a rod, arranged concentrically inside the tube, which are electrically connected at one end. One of the arms of the thermocouple consists essentially of boron carbide formed from self bonding boron carbide by pressureless sintering. Prefabricated sleeves of high-purity, boron-oxide-free hexagonal boron nitride are used between the arms of the thermocouple as spacers. Only the end of the arm of the thermocouple constructed as a rod is secured in an electrically conductive connecting piece and the arm is freely mobile in the direction towards the cold junction. As the material for the arm of the thermocouple constructed as a rod, there can be used, for example, boron carbide having a coarse-grained structure and a density of from 60 to 80% TD, which has been manufactured from boron carbide powder having bimodal particle size distribution by means of extrusion, followed by pressureless sintering at from 2000.degree. to 2250.degree. C.The thermoelement can also be manufactured in one operation by means of pressureless sintering of the boron carbide powder in situ. Such a thermoelement comprises, for example, a flexible graphite cord for the arm of the thermocouple constructed as a rod, a boron-nitride envelope and a boron-carbide casing, the envelope and casing having been formed from powders sintered in situ without pressure.

摘要翻译： 本发明是一种改进的元件，其包括石墨/碳化硼热电偶，其臂构造为管和杆，同心地布置在管内，其一端电连接。 热电偶的一个臂基本上由通过无压烧结自结合碳化硼形成的碳化硼组成。 使用高纯度，不含氧化硼的六方氮化硼的预制套筒作为间隔件在热电偶的臂之间使用。 只有构造为杆的热电偶的臂的端部固定在导电连接件中，并且臂可以在朝向冷端的方向上自由移动。 作为构造为棒的热电偶的臂的材料，可以使用例如具有粗颗粒结构和密度为60至80％TD的碳化硼，其由具有 通过挤出进行双峰粒度分布，然后在2000〜2250℃进行无压烧结。也可以通过在原位无碳烧结碳化硼粉末的一次操作中制造热电偶。 这样的热电元件例如包括用作用作棒的热电偶的臂的柔性石墨帘线，氮化硼外壳和碳化硼外壳，外壳和壳体由没有压力原位烧结的粉末形成。

公开(公告)号：US4560668A

公开(公告)日：1985-12-24

申请号：US648608

申请日：1984-09-07

申请人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth

发明人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth

IPC分类号： C04B35/565 ,  C04B35/575 ,  C04B35/584 ,  C04B35/593 ,  C04B35/56 ,  C04B35/58

CPC分类号： C04B35/575 ,  C04B35/593

摘要： The invention is substantially pore-free shaped articles consisting essentially of polycrystalline silicon nitride and polycrystalline silicon carbide in the form of a homogeneous microstructure having grain sizes of not more than 10 .mu.m manufactured from mixtures of Si.sub.3 N.sub.4 powder and SiC powder in a weight ratio of from 5:95 to 95:5 without the concomitant use of sintering aids by isostatic hot pressing in a vacuum-sealed casing at temperatures of from 1800.degree. to 2200.degree. C. and a pressure of from 100 to 400 MPa.

摘要翻译： 本发明是基本上由多晶氮化硅和多晶碳化硅组成的基本上无孔的成形制品，其形式为均匀微结构，其晶粒尺寸不超过10微米，由Si 3 N 4粉末和SiC粉末的混合物制成，重量比为 从5:95至95:5，而在1800至2200℃的温度和100至400MPa的压力下，在真空密封的壳体中通过等静压热压同时使用烧结助剂。

公开(公告)号：US4381931A

公开(公告)日：1983-05-03

申请号：US304948

申请日：1981-09-23

申请人： Klaus Hunold ,  Klaus Reinmuth ,  Alfred Lipp

发明人： Klaus Hunold ,  Klaus Reinmuth ,  Alfred Lipp

IPC分类号： B22F3/14 ,  B22F3/12 ,  B22F3/15 ,  C04B35/64 ,  C04B35/645

CPC分类号： B22F3/1241 ,  B22F3/1225 ,  C04B35/6455

摘要： The invention relates to a process for the manufacture of substantially pore-free shaped articles of polycrystalline material such as aluminium oxide, titanium boride, silicon nitride or silicon carbide, in which pulverulent materials or preformed articles having pores open towards the surface, in a vacuum-tight sealed glass casing that has a viscosity of less than 10.sup.6 Pas at the pressing temperature employed, are isostatically hot-pressed in a high-pressure autoclave using an inert gas as pressure-transfer medium. By being embedded in a flowable pile or by having a layer applied to them in the form of a suspension, the glass-encased powders or articles are brought into contact with a heat-resistant pulverulent material that, upon softening of the glass casing, penetrates into the surface of the glass of reacts with it, with the result that the glass casing is reinforced from the outside at the pressing temperature. As pulverulent materials, there may be used titanium boride, graphite, SiC or boron nitride, which do not react with the glass casing, or glass powder or silica, which react with the glass casing to form a glass melt of at least the same viscosity as, or of a higher viscosity than, the glass casing.

摘要翻译： 本发明涉及一种用于制造基本上无孔的成形制品的多晶材料，例如氧化铝，硼化钛，氮化硅或碳化硅，其中粉末材料或具有孔朝向表面开口的预制制品在真空中 在所使用的压制温度下粘度小于106Pa·s的密封玻璃外壳在使用惰性气体作为压力传递介质的高压高压釜中进行等静压热压。 通过嵌入可流动的桩中或通过以悬浮液的形式施加到其上的层，使玻璃包裹的粉末或制品与耐热粉末材料接触，所述耐热粉末材料在玻璃套管的软化时穿透 玻璃表面与玻璃反应，结果玻璃外壳在压制温度下从外部增强。 作为粉状材料，可以使用不与玻璃外壳反应的硼化钛，石墨，SiC或氮化硼，或与玻璃外壳反应的玻璃粉末或二氧化硅，以形成至少相同粘度的玻璃熔体 或者比玻璃外壳高的粘度。

公开(公告)号：US4528120A

公开(公告)日：1985-07-09

申请号：US601986

申请日：1984-04-19

申请人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth

发明人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth

IPC分类号： C04B35/565 ,  C04B35/58 ,  C04B35/581 ,  C04B35/583 ,  C04B35/584 ,  C04B35/645 ,  C23C14/24 ,  H01B1/04

CPC分类号： C04B35/5607 ,  C04B35/5611 ,  C04B35/565 ,  C04B35/58064 ,  C04B35/58071 ,  C04B35/58078 ,  C04B35/581 ,  C04B35/583 ,  C04B35/632 ,  C04B35/645 ,  C04B35/6455 ,  C23C14/243 ,  Y10T428/12458

摘要： The invention is refractory, electrically conductive, mixed materials based on hexagonal boron nitride and at least one electrically conductive component such as titanium boride and zirconium boride, and having a density of at least about 95% of the theoretical density and nondirection-dependent properties, which have been manufactured from powder mixtures that are practically free of oxygen and metal and comprisefrom about 10 to 60% by weight of boron nitride,from about 0 to 60% by weight of aluminum nitride and/or silicon nitride, andfrom about 30 to 70% by weight of an electrically conductive component,without the concomitant use of sintering aids by means of isostatic hot pressing in a vacuum-tight casing at temperatures of from about 1400.degree. to 1700.degree. C. and under a pressure of from about 100 to 300 MPa. The powder mixtures are pre-densified to form green bodies in block form and are then introduced into casings or coated with a material forming a vacuum-tight casing. The pre-densified green bodies in the vacuum-tight casing are then subjected to the isostatic hot-pressing process in a high-pressure autoclave, using an inert gas such as argon, as pressure-transmission medium. The article formed from the mixed materials are used to manufacture evaporation boats for the vacuum evaporation of metals.

摘要翻译： 本发明是基于六方氮化硼和至少一种导电组分如硼化钛和硼化锆的耐火材料，导电的混合材料，并且具有至少约95％的理论密度和非方向依赖性质的密度， 其由实际上不含氧和金属的粉末混合物制成，并且包含约10至60重量％的氮化硼，约0至60重量％的氮化铝和/或氮化硅，以及约30 至70重量％的导电组分，而不伴随使用烧结助剂，通过在真空密封的壳体中通过在约1400℃至1700℃的温度和约100℃的压力下的等静压热压 至300MPa。 将粉末混合物预先致密化以形成块状的生坯，然后将其引入壳体中或涂覆形成真空密封套管的材料。 然后将真空密封的外壳中的预致密生坯在高压高压釜中使用惰性气体如氩气进行等静压热压作为压力传递介质。 由混合材料制成的制品用于制造用于金属真空蒸发的蒸发舟。

公开(公告)号：US4634640A

公开(公告)日：1987-01-06

申请号：US646627

申请日：1984-08-31

申请人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth

发明人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth

IPC分类号： C04B35/583 ,  C04B35/645 ,  B32B5/16 ,  B32B15/02 ,  B32B21/02 ,  B32B27/02

CPC分类号： C04B35/6455 ,  C04B35/583

摘要： The invention is a shaped article of boron nitride having a density of at least 95% of the theoretical density which consists of polycrystalline hexagonal boron nitride in the form of a homogeneous isotropic microstructure and which has been manufactured from pure boron nitride powder without the concomitant use of sintering aids by isostatic hot-pressing in a vacuum-tight casing at temperatures of from about 1200.degree. to 1500.degree. C. under a pressure of from about 50 to 300 MPa. Boron nitride powders having a free boric oxide content of not more than 1.0% by weight and having a specific surface area of from 5 to 30 m.sup.2 /g are used as starting material. The powders either are filled into prefabricated casings consisting of steel or glass and densified by vibration or are preshaped to form green bodies having pores open to the surface and then placed in prefabricated casings or coated with a material which forms a vacuum-tight casing. The powders or the preshaped green bodies in the vacuum-tight casings are then subjected to an isostatic hot-pressing process in a high-pressure zone using an inert gas such as argon or nitrogen, as the pressure-transfer medium.

摘要翻译： 本发明是氮化硼的成型制品，其密度至少为理论密度的95％，由均匀的各向同性微观结构形式的多晶六方氮化硼组成，并且由纯氮化硼粉末制造而不伴随使用 的烧结助剂通过在约1200至1500℃的温度下在约50至300MPa的压力下在真空密封的壳体中等静压热压。 使用游离氧化硼含量为1.0重量％以下，比表面积为5〜30m 2 / g的氮化硼粉末作为起始原料。 将粉末填充到由钢或玻璃组成的预制外壳中并通过振动而致密化，或者被预成型形成具有通向表面的孔的生坯，然后放置在预制外壳中或涂覆有形成真空密封外壳的材料。 作为压力传递介质，将真空密封的壳体中的粉末或预成形的生坯在高压区域中进行等静压热压工艺，使用惰性气体如氩气或氮气进行。

公开(公告)号：US4564601A

公开(公告)日：1986-01-14

申请号：US646022

申请日：1984-08-29

申请人： Jochen Kriegesmann ,  Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth ,  Karl A. Schwetz

发明人： Jochen Kriegesmann ,  Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth ,  Karl A. Schwetz

IPC分类号： C04B35/565 ,  C04B35/575 ,  C04B35/64 ,  C04B35/645 ,  C04B35/56

CPC分类号： C04B35/575 ,  C04B35/6455

摘要： The invention is substantially pore-free shaped articles which consist essentially of polycrystalline .alpha.- or .beta.-silicon carbide in the form of a single-phase homogeneous microstructure having grain sizes not exceeding 8 .mu.m, and which are manufactured from SiC powder, without the concomitant use of sintering aides, by isostatic hot-pressing in a vacuum-tight casing at temperatures of from about 1900.degree. C. to 2300.degree. C. and at pressures of from about 100 to 400 MPa. The SiC starting materials have .alpha.- and/or .beta.-SiC powders having a total content of metallic impurities not exceeding 0.1% by weight and a particle size of 4 .mu.m and finer.

摘要翻译： 本发明是基本上无孔的成形制品，其基本上由具有不超过8μm的晶粒尺寸的单相均匀组织形式的多晶α-或β-碳化硅组成，并且由SiC粉末制成，没有 伴随使用烧结助剂，通过在真空密封的套管中通过在约1900℃至2300℃的温度和约100至400MPa的压力下等静压热压。 SiC原料具有金属杂质的总含量不超过0.1重量％且粒径为4μm的α和/或β-SiC粉末，并且更细。

公开(公告)号：US4495123A

公开(公告)日：1985-01-22

申请号：US454164

申请日：1982-12-29

申请人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth

发明人： Klaus Hunold ,  Alfred Lipp ,  Klaus Reinmuth

IPC分类号： C04B35/583 ,  C04B35/645 ,  C01B21/06

CPC分类号： C04B35/6455 ,  C04B35/583

摘要： The invention is a shaped article of boron nitride having a density of at least 95% of the theoretical density which consists of polycrystalline hexagonal boron nitride in the form of a homogeneous isotropic microstructure and which has been manufactured from pure boron nitride powder without the concomitant use of sintering aids by isostatic hot-pressing in a vacuum-tight casing at temperatures of from about 1200.degree. to 1500.degree. C. under a pressure of from about 50 to 300 MPa. Boron nitride powders having a free boric oxide content of not more than 1.0% by weight and having a specific surface area of from 5 to 30 m.sup.2 /g are used as starting material. The powders either are filled into prefabricated casings consisting of steel or glass and densified by vibration or are preshaped to form green bodies having pores open to the surface and then placed in prefabricated casings or coated with a material which forms a vacuum-tight casing. The powders or the preshaped green bodies in the vacuum-tight casings are then subjected to an isostatic hot-pressing process in a high-pressure zone using an inert gas such as argon or nitrogen, as the pressure-transfer medium.

摘要翻译： 本发明是氮化硼的成型制品，其密度至少为理论密度的95％，由均匀的各向同性微观结构形式的多晶六方氮化硼组成，并且由纯氮化硼粉末制造而不伴随使用 的烧结助剂通过在约1200至1500℃的温度下在约50至300MPa的压力下在真空密封的壳体中等静压热压。 使用游离氧化硼含量为1.0重量％以下，比表面积为5〜30m 2 / g的氮化硼粉末作为起始原料。 将粉末填充到由钢或玻璃组成的预制外壳中并通过振动而致密化，或者被预成型形成具有通向表面的孔的生坯，然后放置在预制外壳中或涂覆有形成真空密封外壳的材料。 作为压力传递介质，将真空密封的壳体中的粉末或预成形的生坯在高压区域中进行等静压热压工艺，使用惰性气体如氩气或氮气进行。

公开(公告)号：US4467043A

公开(公告)日：1984-08-21

申请号：US507932

申请日：1983-06-23

申请人： Jochen Kriegesmann ,  Alfred Lipp ,  Klaus Reinmuth

发明人： Jochen Kriegesmann ,  Alfred Lipp ,  Klaus Reinmuth

IPC分类号： C04B35/565 ,  C04B35/575 ,  C04B35/36

CPC分类号： C04B35/575

摘要： The invention relates to dense shaped articles of polycrystalline .alpha.-silicon carbide containing from 0.1 to 0.4%, by weight, of aluminum and optionally, a small amount of nitrogen and/or phosphorus, having a homogeneous virtually single-phase microstructure. The additional constituents are substantially in the form of a solid solution in the .alpha.-SiC lattice. The shaped articles are distinguished by flexural strength of at least 600 N/mm.sup.2 up to 1450.degree. C. and low subcritical crack propagation under mechanical stress. The fracture mechanism is trans granular up to at least 1450.degree. C. The shaped articles are manufactured by simultaneously shaping and hot pressing pulverulent .alpha.-silicon carbide containing a small amount of an aluminum-containing additive, such as aluminum powder, aluminum nitride and/or aluminum phosphide, at temperatures between 1850.degree. C. and 2300.degree. C. under a pressure of at least 100 bar (10 MPa).

摘要翻译： 本发明涉及包含0.1至0.4重量％的铝和任选的少量氮和/或磷的多晶α-碳化硅的致密成型制品，其具有均匀的实质上单相微观结构。 附加组分基本上是α-Si晶格中固溶体的形式。 成形制品的特征在于至少600N / mm 2至1450℃的弯曲强度和在机械应力下的低亚临界裂纹扩展。 断裂机理是反式颗粒至多至1450℃。成型制品通过同时成型和热压含有少量含铝添加剂的粉末状α-碳化硅，如铝粉，氮化铝和/ 或磷化铝，在至少100巴（10MPa）的压力下，在1850℃至2300℃的温度下进行。