CN102325729B - 具有高氧化锆含量的耐火产物 - Google Patents
具有高氧化锆含量的耐火产物 Download PDFInfo
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Abstract
本发明涉及一种熔铸耐火产物,其包括以下重量百分比的各氧化物且这些氧化物总计为100%:ZrO2+Hf2O:补足余数至100%;SiO2:7.0%至11.0%;Al2O3:0.2%至0.7%;Na2O+K2O:<0.10%;B2O3:0.3%至1.5%;CaO+SrO+MgO+ZnO+BaO:<0.4%;P2O5<0.15%;Fe2O3+TiO2:<0.55%;其它氧化物物质:<1.5%;该产物具有重量含量小于或等于1.0%的选自Nb2O5、Ta2O5及其混合物的掺杂剂,Al2O3重量含量/B2O3重量含量,即“A/B”比小于或等于2.0,不包括呈220×450×150mm3的块或直径为30mm且高度为30mm的圆柱棒状的熔铸产物,该熔铸产物以各氧化物的质量百分比计具有以下化学组成:表格(I)。本发明可用于玻璃熔融炉。
Description
技术领域
本发明涉及一种具有高氧化锆含量的新颖熔铸耐火产物。
背景技术
在耐火产物中,熟知用于构建玻璃熔融炉的熔铸产物与烧结产物之间存在区别。
不同于烧结产物,熔铸产物最常包括连接结晶晶粒的晶粒间玻璃相。烧结产物及熔铸产物所造成的问题不同,因此解决这些问题所采用的技术解决方案一般亦不同。因此,一种开发用于制造烧结产物的组成物显然不适用于制造熔铸产物,反之亦然。
熔铸产物常被称为电熔合产物,其利用在电弧炉中熔融合适原料的混合物或利用适用于这些产物的任一其它技术而获得。熔料随后被浇铸至模具中,且所得产物接着经受控制冷却循环以恢复室温而不破裂。本领域技术人员亦将此项操作称为“退火”。
在熔铸产物中,具有高氧化锆含量,亦即包括按重量计超过85%的氧化锆(ZrO2)的电熔合产物的显著特性在于其极高耐蚀性,而不会使所制造的玻璃着色且不会产生缺陷。
惯常地,具有高氧化锆含量的熔铸产物亦包括氧化钠(Na2O),以避免由存在于产物中的氧化锆与二氧化硅形成锆石。当锆石的形成伴随有约20%的体积减小时,其实际上为有害的,由此在裂痕起点处产生机械应力。
由Saint-Gobain SEFPRO制造及销售且涵盖于专利EP-B-403 387中的产品ER-1195现今广泛用于玻璃熔融炉中。其化学组成包含约94%的氧化锆、4%至5%的二氧化硅、约1%的氧化铝、0.3%的氧化钠及按重量计小于0.05%的P2O5。其为用于玻璃制造炉的典型的具有高氧化锆含量的产物。
FR 2 701 022描述具有高氧化锆含量的熔铸产物,这些熔铸产物含有按重量计为0.05至1.0%的P2O5及按重量计为0.05至1.0%的三氧化二硼B2O3。该产物具有高电阻率。由此,其可能宜稳定玻璃电熔融期间的耗电量且避免在耐火产物中出现任何会导致其快速降解的短路问题。实际上,在玻璃电熔融期间,部分电流通过这些耐火产物。增加这些耐火产物的电阻率能够使能够流经其的电流量减少。
WO 2005 068393描述具有高氧化锆含量的熔铸产物,这些熔铸产物具有高电阻率,同时将BaO、SrO、MgO、CaO、P2O5、Na2O及K2O含量降至最低。针对氧化铝含量介于0.9与2.5%之间,这些产物含有按重量计0.1至1.2%的B2O3。
JP 63 285173描述具有高氧化锆含量的熔铸产物,针对二氧化硅含量小于6.5%,这些熔铸产物具有优良电阻率及抗破裂性。
目前开发的高质量玻璃,具体为用于LCD型平面屏幕的玻璃板,会增加对玻璃熔融炉的耐火产物的要求。具体而言,需要一种无须借助于掺杂剂而具有进一步增强的电阻率的耐火产物。
本发明旨在满足此需要。
发明内容
更具体地说,本发明涉及一种熔铸耐火产物,其包含以下质量百分比的各氧化物且这些氧化物的总量为100%:
Al2O3质量含量/B2O3质量含量,即“A/B”比小于或等于2.0。
如稍后可见,本发明者已意外地发现,具有该组成的本发明产物可能具有改善的电阻率。
本发明的耐火产物可能接着包括一或多个以下可选特征:
-Al2O3质量含量/B2O3质量含量,即“A/B”比小于或等于1.8,优选小于1.5,优选小于1.2,优选小于1.0,小于0.8或甚至小于0.7。
-Al2O3质量含量/B2O3质量含量,即“A/B”比大于0.1,或甚至大于0.2,或甚至大于0.3。
-二氧化硅(SiO2)的质量含量小于或等于11.0%,或甚至小于或等于10.0%,或甚至小于或等于9.5%。
-二氧化硅(SiO2)的质量含量大于或等于7.5%,大于或等于7.7%,或甚至大于或等于8.0%。
-氧化铝(Al2O3)的质量含量小于或等于0.7%,或甚至小于或等于0.6%,或甚至小于或等于0.5%。
-Al2O3的质量含量大于或等于0.25%,大于或等于0.3%。在一具体实例中,此含量大于或等于0.4%。
-氧化铝(Al2O3)仅以杂质形式存在。
-(Na2O+K2O)的质量含量小于或等于0.05%,或甚至小于或等于0.03%。
-B2O3的质量含量大于或等于0.35%,或甚至大于或等于0.4%,或甚至大于或等于0.5%。
-B2O3的质量含量小于或等于1.2%,或甚至小于或等于1.0%,或甚至小于或等于0.80%,或小于或等于0.75%,或小于或等于0.70%,或小于或等于0.65%。
-P2O5的质量含量小于或等于0.05%。
-氧化铁及/或氧化钛及/或氧化钙及/或氧化锶及/或氧化钡及/或氧化镁及/或氧化锌及/或五氧化二磷仅以杂质形式存在。
-氧化铁及/或氧化钛Fe2O3+TiO2的质量含量小于0.4%,优选小于0.3%,优选小于0.2%。
-氧化钙及/或氧化锶及/或氧化钡及/或氧化镁及/或氧化锌的质量含量小于0.2%,优选小于0.1%。
-氧化钙及/或氧化锶及/或氧化钡及/或氧化镁及/或氧化锌CaO+SrO+BaO+MgO+ZnO的总质量含量小于0.3%,优选小于0.2%。
-“其它氧化物物质”的总质量含量小于1.0%。
-“其它氧化物物质”仅由杂质组成,且“其它氧化物物质”的总质量含量小于0.6%,小于0.5%,或甚至小于0.3%。
-产物包括质量含量大于或等于0.1%,优选大于或等于0.2%,优选大于或等于0.25%及/或小于或等于1.3%,小于或等于1.0%,优选小于或等于0.9%,更优选小于或等于0.6%的选自Nb2O5、Ta2O5及其混合物的掺杂剂。
-ZrO2/(Nb2O5+Ta2O5)的莫耳比介于200与350之间。
-ZrO2/(Nb2O5+Ta2O5)的莫耳比大于250。
-掺杂剂Ta2O5的质量含量大于或等于0.1%,优选大于或等于0.2%,及/或小于或等于1.2%,优选小于或等于0.6%。
-掺杂剂Nb2O5的质量含量大于或等于0.1%,优选大于或等于0.2%,及/或小于或等于1.0%,优选小于或等于0.6%。
-在一具体实例中,Nb2O5+Ta2O5的总质量含量小于或等于0.6%。
-二氧化硅(SiO2)的质量含量大于或等于8.0%且小于或等于10.0%,且选自Nb2O5、Ta2O5及其混合物的掺杂剂的质量含量小于或等于0.6%。
-三氧化二钇(Y2O3)的质量含量小于或等于1%,优选小于0.5%,更优选小于0.3%,或甚至小于0.2%。
-在一具体实例中,BaO含量小于0.10%,或实质上为零。
-本发明不包括专利申请第WO 2007 099 253号、第PCT/FR2008/051516号及第PCT/FR2008/051515号(及同族专利申请)中所公开的产物,且尤其不包括这些专利申请的实例中的产物。
-本发明不包括下列呈220×450×150mm3的块状或呈直径为30mm且高度为30mm的圆柱棒状的产物,其组成由以下质量百分比的各氧化物提供:
ZrO2 | SiO2 | B2O3 | Al2O3 | Nb2O5 | Ta2O5 | Y2O3 | BaO |
90.3 | 7.1 | 0.6 | 0.79 | 0.33 | 0.76 | 0.2 | |
91.1 | 7.5 | 0.6 | 0.44 | 0.17 | 0.13 | ||
90 | 8.1 | 0.41 | 0.54 | 0.74 | 0.20 | ||
89.2 | 8.3 | 0.49 | 0.8 | 0.31 | 0.7 | 0.2 | |
89.8 | 8.4 | 0.48 | 0.44 | 0.66 | 0.2 | ||
89.3 | 8.9 | 0.49 | 0.47 | 0.71 | 0.2 | ||
88.6 | 9.3 | 0.54 | 0.5 | 0.76 | 0.2 | 0.13 | |
87.6 | 10.2 | 0.53 | 0.53 | 0.8 | 0.19 | 0.1 | |
87.4 | 10.8 | 0.89 | 0.54 | 0.2 | 0.18 | 0.03 | |
87.3 | 11.2 | 0.6 | 0.54 | 0.16 | 0.17 | 0.02 | |
90.2 | 7.4 | 0.9 | 0.3 | 1.2 |
-在一实施例中,所有具有上表中的组成的产物皆不包括在内,无论其为何种形式。
-在一实施例中,所有组成接近于上表中的至少一种组成的产物皆不包括在内。在不考虑第一种组成的相关组分的情况下,当第一种组成中该组分的含量与第二种组成中该组分的含量的绝对差异以质量百分比计小于0.10%时,认为第一种组成“接近”于第二种组成。
在一优选实施例中,SiO2≤11.0%,优选SiO2≤10.0%,且Ta2O5+Nb2O5≤1.0%,优选Nb2O5≤0.6%。
更优选地,
-SiO2≤10.0%且Ta2O5+Nb2O5≤1.0%,其中Nb2O5≤0.6%,且
-Na2O+K2O≤0.05%,或甚至Na2O+K2O≤0.03%,且
-CaO+SrO+MgO+ZnO+BaO<0.3%,或甚至CaO+SrO+MgO+ZnO+BaO<0.2%,且
-BaO<0.1%,且
-Fe2O3+TiO2<0.3%,且
-Y2O3<0.3%。
本发明还涉及一种制造本发明的耐火产物的方法,其包含以下连续步骤:
a)混合原料以获得初始负载;
b)熔融该初始负载直至获得熔料;
c)浇铸该熔料且通过冷却使其凝固,以获得耐火产物,
该方法的显著之处在于,这些原料经选择使得该耐火产物符合本发明。
优选地,系统且有条理地添加需要极少含量的氧化物,尤其是ZrO2、SiO2、B2O3或这些氧化物的前体。优选地,考虑惯常将这些氧化物视为杂质的其它氧化物来源中这些氧化物的含量。
优选控制冷却,以便优选以每小时小于20℃的速率进行冷却,优选以每小时约10℃的速率进行冷却。
本发明还涉及一种包括本发明的耐火产物或根据本发明方法制造的耐火产物或能够根据本发明方法制造的耐火产物的玻璃熔融炉,具体而言,该玻璃熔融炉意欲在一定区域中与熔融玻璃接触。在本发明的炉中,耐火产物宜成为通过熔融、尤其通过电熔融制备玻璃的容器的一部分,在该容器中耐火产物能够在1,200℃以上的温度下开始与熔融玻璃接触。
定义
氧化物质量含量指根据通常工业惯例,各表示为最稳定氧化物的对应化学元素的整体含量;因此,次氧化物及可能存在的氮化物、氮氧化物、碳化物、碳氧化物、碳氮化物或甚至上述元素中的金属物质亦包括在内。
“熔料(molten material)”为液体块,为保持其形状,应将其容纳于容器中。熔料可能含有少量固体粒子,但固体粒子的量不足以使其能够构成该块状物。
“杂质(impurities)”意指偶然但亦必然与原料一起引入或由与这些组分反应所产生的不可避免的组分。杂质非所需组分,而仅为容许存在的组分。例如,铁、钛、钒及铬的氧化物、氮化物、氮氧化物、碳化物、碳氧化物、碳氮化物及金属物质中的部分化合物为杂质。
除非另外指明,否则所描述且所保护的产物中所有氧化物的含量均为这些氧化物的质量百分比。
具体实施方式
在本发明的具有高氧化锆(ZrO2)含量的熔铸产物中,有可能满足以下需求,即具有高耐蚀性,而不会使所制造的玻璃着色或产生对此玻璃的质量有害的缺陷。
在通过熔融而获得的产物中,HfO2无法以化学方法与ZrO2分离。因此,在此类产物的化学组成中,ZrO2+HfO2表示该两种氧化物的总含量。然而,根据本发明,初始负载中的HfO2并非特意添加的。因此,HfO2仅表示痕量二氧化铪,该氧化物始终以一般小于2%的含量天然存在于氧化锆来源中。因此,为清晰起见,可由ZrO2+HfO2或由ZrO2或另外由“氧化锆含量”表示氧化锆含量及二氧化铪微含量。
在本发明产物中,二氧化铪HfO2含量小于或等于5%,一般小于或等于2%。
二氧化硅SiO2的存在尤其会导致形成晶粒间玻璃相,晶粒间玻璃相在氧化锆发生可逆性同素异形变化期间(亦即,自单斜晶相变化为四方晶相时)能够有效地调节其体积变化。在存在质量含量大于7.0%的二氧化硅(SiO2)时,可获得高电阻率。
另一方面,所添加的二氧化硅不应超过12.5%,因为添加二氧化硅会对氧化锆含量造成不利影响且因此可对耐蚀性造成不利影响。另外,过高二氧化硅含量可通过释放石块(由于产物丧失内聚力而产生的耐火产物碎片)而在玻璃中产生缺陷,这在应用时被视为不良行为。
氧化铝的存在会促进稳定玻璃相形成且会改善产物在模具中的可铸性。含量过高会导致玻璃相不稳定(形成晶体),其对可行性产生消极影响,尤其在存在三氧化二硼时如此。因此,氧化铝质量含量应保持低于0.8%。
在本发明产物中,认为氧化物Na2O及K2O具有类似效应。
Na2O及K2O氧化物对电阻率具有反效应。因此,Na2O+K2O的质量含量应小于0.1%。
B2O3质量含量的存在比例使得Al2O3质量含量/B2O3质量含量(即A/B比)小于或等于2,由此增加电阻率。
根据本发明,Fe2O3+TiO2的质量含量小于0.55%且P2O5的质量含量小于0.15%,优选小于0.10%,更优选小于0.05%。实际上,已知这些氧化物为有害的,且其作为杂质与原料一起引入时的含量应优选限于痕量。
“其它氧化物物质”为以上未列出的物质,亦即,除ZrO2、Hf2O、SiO2、Al2O3、Na2O、K2O、B2O3、CaO、SrO、BaO、MgO、ZnO、P2O5、Fe2O3及TiO2以外的物质。具体而言,Nb2O5及Ta2O5属于“其它氧化物物质”。
在一实施例中,“其它氧化物物质”限于非特别需要存在且一般以杂质形式存在于原料中的物质。
在另一实施例中,“其它氧化物物质”亦可能包含有利地存在的物质。因此,在一实施例中,产物有利地包括至少0.1%、优选至少0.2%的可能进一步改良电阻率的掺杂剂,例如Nb2O5、Ta2O5或其混合物。然而,掺杂剂质量含量优选小于或等于1.0%,优选小于或等于0.9%,更优选小于或等于0.6%。
在一实施例中,“其它氧化物物质”既不包括Nb2O5,亦不包括Ta2O5(产物不含这些氧化物)。
惯常地,在熔铸产物中,氧化物占产物质量的98.5%以上,99%以上,或实质上100%。上述情况亦适用于本发明的产物。
本发明产物惯常可根据下述步骤a)至c)来制造:
a)混合原料以形成初始负载;
b)熔融该初始负载直至获得熔料;
c)利用冷却使该熔料凝固,以获得本发明的耐火产物。
在步骤a)中,原料经选择以保证成品中氧化物的含量。
在步骤b)中,优选借助于不会引起任何还原的较长电弧与促进产物再氧化的混合的组合作用来实现熔融。
为将具有金属态样的生料粒的形成减至最少且为避免在最终产物中形成裂痕或裂纹,优选在氧化条件下进行熔融。
优先使用法国专利第1 208 577号及其增补案第75893号及第82310号中所述的长弧熔融方法。
该方法由以下步骤组成:使用电弧炉,其弧存在于负载与至少一个远离该负载的电极之间;及调节弧长度使得其还原作用减少至最低程度,同时在熔融浴上方保持氧化气氛且借由弧本身的作用,或借由使氧化气体(例如空气或氧气)在浴中鼓泡或另外借由向浴中添加释放氧气的物质(诸如过氧化物或硝酸盐)来混合该浴。
具体而言,可在2,300℃以上的温度下,优选在介于2,400℃与2,500℃之间的温度下进行熔融。
在步骤c)中,优选以每小时小于20℃的速率,优选以每小时约10℃的速率进行冷却。
由此制造的本发明产物由玻璃相所围绕的氧化锆晶粒组成。以质量百分比计超过80%、超过90%、超过99%或实质上100%的氧化锆可为单斜晶的。以基于玻璃相的质量百分比计,玻璃相可包括超过50%或甚至超过70%的二氧化硅、在5%与20%之间的B2O3及在1%与20%之间的氧化铝。二氧化硅、B2O3及氧化铝可占玻璃相质量的95%以上、97%以上或实质上100%。
亦可应用任何基于意欲应用于玻璃熔融炉中的氧化锆来制造熔合产物的常规方法,其限制条件为初始负载的组成允许获得组成符合本发明产物的组成的产物。
实例
给出以下非限制性实例以达成说明本发明的目的。
在这些实例中,使用以下原料:
-氧化锆,主要含有平均质量为98.5%的ZrO2+HfO2、0.2%的SiO2及0.02%的Na2O;
-锆砂,含有33%的二氧化硅;
-三氧化二硼,纯度超过99%。
在电弧炉中根据标准熔融方法熔融原料,随后浇铸熔料以获得规格为220mm×450mm×150mm的块。
实例1对应于由Saint-Gobain SEFPRO销售的产品ER1195,且为参考物。
对于所有所得产物而言,结晶分析显示由通常包括超过70%的二氧化硅的玻璃相围绕的单斜晶氧化锆晶体。在玻璃相中再次发现二氧化硅以及除氧化锆以外的其它氧化物物质全体。
表1给出所得产物的化学分析;此分析为平均整体化学分析,以质量百分比形式给出。
在下表1中,*指示该实例不在本发明内,空方框对应于质量含量小于或等于0.05%。用“其它氧化物物质”补足余数至100%。
自不同的所得示例性块上取出直径为30mm且高度为30mm的圆柱棒产物。分别使这些棒在1,500℃或1,600℃下以100赫兹的频率经受1伏特电位差,以分别进行电阻率测量“R1500”及“R1600”。
表1
实例6至9的比较证实,在二氧化硅含量实质上恒定且不存在Na2O的情况下,小于2.0或甚至小于1.5且甚至小于0.8的A/B比会引起正效应,实例9为优选实例。
结果亦显示,尽管不存在掺杂剂,但本发明的测试产物仍具有改善的电阻率。
为证实这些最初结果,本发明者在熔合的1kg玻璃相块上继续进行其它电阻率测量。分别使这些块在1,500℃或1,600℃下以2,500赫兹的频率经受1伏特电位差,以分别进行电阻测率量“R1500”及“R1600”。结果概述于表2中。
这些测试证实A/B比的重要性。
表2
表2进一步显示,在A/B比为0.6的实例12中,针对R1500所获得的最佳效能类似于针对R1600所获得的最佳效能。
当然,本发明不限于所描述且说明的具体实施例,这些具体实施例作为说明性及非限制性实例提供。
Claims (15)
1.一种熔铸耐火产物,其包括以下质量百分比的各氧化物且这些氧化物总计为100%:
选自Nb2O5、Ta2O5及其混合物的掺杂剂的质量含量小于或等于1.0%;
Al2O3质量含量/B2O3质量含量,即“A/B”比小于或等于2.0;
不包括呈220×450×150mm3的块或直径为30mm且高度为30mm的圆柱棒状的熔铸产物,该熔铸产物以各氧化物的质量百分比计具有以下化学组成:
。
2.如权利要求1所述的产物,包括质量含量大于或等于0.1%的所述掺杂剂。
3.如权利要求1所述的产物,包括质量含量小于或等于0.6%的所述掺杂剂。
4.如权利要求1所述的产物,包括质量含量小于或等于0.6%的Nb2O5。
5.如权利要求1所述的产物,既不包括Nb2O5,也不包括Ta2O5。
6.如权利要求1所述的产物,其中二氧化硅SiO2的质量含量大于或等于8.0%。
7.如权利要求1所述的产物,其中B2O3的质量含量大于或等于0.5%。
8.如权利要求1所述的产物,其中B2O3的质量含量小于或等于1.0%。
9.如权利要求8所述的产物,其中B2O3的质量含量小于或等于0.8%。
10.如权利要求1的产物,其中Na2O+K2O的质量含量大于或等于0.05%,氧化铁及/或氧化钛Fe2O3+TiO2的质量含量小于0.4%,P2O5的质量含量小于或等于0.05%,且“其它氧化物物质”的总质量含量小于0.6%。
11.如前述权利要求中任一项所述的产物,其中该A/B比小于1.5。
12.如权利要求11的产物,其中该A/B比小于0.8。
13.根据权利要求1所述的产物,其中,Na2O+K2O的质量含量小于0.03%。
14.根据权利要求1所述的产物,其中,Fe2O3+TiO2的含量小于0.3%。
15.一种熔铸耐火产物,包括以下质量百分比的各氧化物且这些氧化物总计为100%:
Al2O3质量含量/B2O3质量含量,即“A/B”比小于或等于2.0,Nb2O5及Ta2O5的含量使得:
Nb2O5≤0.6%,
Nb2O5+Ta2O5≤1.0%;
不包括呈220×450×150mm3的块或直径为30mm且高度为30mm的圆柱棒状的熔铸产物,该熔铸产物以各氧化物的质量百分比计具有以下化学组成:
。
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FR0951189A FR2942468B1 (fr) | 2009-02-25 | 2009-02-25 | Produit refractaire a forte teneur en zircone. |
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PCT/IB2010/050816 WO2010097769A1 (fr) | 2009-02-25 | 2010-02-24 | Produit refractaire a forte teneur en zircone |
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FR2953825B1 (fr) * | 2009-12-16 | 2013-12-20 | Saint Gobain Ct Recherches | Produit refractaire a forte teneur en zircone. |
FR2955578B1 (fr) * | 2010-01-28 | 2014-06-13 | Saint Gobain Ct Recherches | Produit refractaire a forte teneur en zircone |
JP5718599B2 (ja) * | 2010-08-20 | 2015-05-13 | 株式会社ノリタケカンパニーリミテド | ジルコニア焼結体、並びにその焼結用組成物及び仮焼体 |
FR2969145B1 (fr) * | 2010-12-16 | 2013-01-11 | Saint Gobain Ct Recherches | Produit refractaire a haute teneur en zircone. |
FR2986227B1 (fr) * | 2012-01-27 | 2014-01-10 | Saint Gobain Isover | Procede de production de laine minerale |
EP2835364B1 (en) * | 2012-04-06 | 2020-06-10 | AGC Inc. | High zirconia fused cast refractory |
FR2996843B1 (fr) * | 2012-10-15 | 2020-01-03 | Saint-Gobain Centre De Recherches Et D'etudes Europeen | Produit d'oxyde de chrome. |
JP5763823B1 (ja) * | 2014-10-07 | 2015-08-12 | サンゴバン・ティーエム株式会社 | 高ジルコニア電気溶融鋳造耐火物 |
JP5806424B1 (ja) * | 2015-02-02 | 2015-11-10 | サンゴバン・ティーエム株式会社 | 高電気抵抗高ジルコニア電気溶融鋳造耐火物 |
FR3032963A1 (fr) * | 2015-02-20 | 2016-08-26 | Saint Gobain Ct Recherches | Produit fondu a forte teneur en zircone |
US20190169073A1 (en) * | 2016-05-20 | 2019-06-06 | Corning Incorporated | Purified ceramic materials and methods for making the same |
CN114394842A (zh) * | 2022-02-18 | 2022-04-26 | 中钢集团洛阳耐火材料研究院有限公司 | 一种烧结的致密高锆砖的制备方法 |
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FR75893E (fr) | 1959-06-11 | 1961-08-18 | Electro Refractaire | Perfectionnements à la fabrication de produits réfractaires électrofondus contenant des oxydes minéraux |
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