CN105849065B - 生产成形耐火陶瓷产品的组合物,生产成形耐火陶瓷产品的方法和成形耐火陶瓷产品 - Google Patents
生产成形耐火陶瓷产品的组合物,生产成形耐火陶瓷产品的方法和成形耐火陶瓷产品 Download PDFInfo
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- 239000000203 mixture Substances 0.000 title claims abstract description 84
- 239000011214 refractory ceramic Substances 0.000 title claims abstract description 48
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 16
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- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 claims description 12
- 229910052727 yttrium Inorganic materials 0.000 claims description 12
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 claims description 11
- 229910052845 zircon Inorganic materials 0.000 claims description 9
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 7
- 229910009474 Y2O3—ZrO2 Inorganic materials 0.000 claims description 7
- 239000006104 solid solution Substances 0.000 claims description 6
- 238000011068 loading method Methods 0.000 claims description 5
- 230000035699 permeability Effects 0.000 claims description 4
- KKCBUQHMOMHUOY-UHFFFAOYSA-N Na2O Inorganic materials [O-2].[Na+].[Na+] KKCBUQHMOMHUOY-UHFFFAOYSA-N 0.000 claims description 3
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 claims description 3
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- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 26
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- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 6
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- 229910001413 alkali metal ion Inorganic materials 0.000 description 1
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- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
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- C04B35/505—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on rare-earth compounds based on yttrium oxide
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Abstract
本发明涉及用于生产成形耐火陶瓷产品的组合物(批料)、用于生产成形耐火陶瓷产品的方法和成形耐火陶瓷产品。
Description
本发明涉及用于生产成形耐火陶瓷产品的组合物(批料)、用于生产成形耐火陶瓷产品的方法和成形耐火陶瓷产品。
如已知,组合物是用于描述可通过陶瓷焙烧由其制成耐火陶瓷产品的一种或多种组分的配混物的术语。对于本发明的目的,术语“耐火陶瓷产品”具体地表示具有高于600℃的工作温度的陶瓷产品,且优选表示根据DIN 51060的耐火材料,也就是说具有大于SK 17的熔锥当量(pyrometric cone equivalent)的材料。熔锥当量可具体根据DIN EN 993-12测定。
已知具体以耐火砖和功能性产品(建筑构件)形式的成形耐火陶瓷产品。
成形耐火陶瓷产品的一种具体应用是其在用于烃热处理的设备中的用途。在用于烃热处理的这类设备中,烃或含有烃的原料经受热处理,以将其转化成不同的材料。
用于热处理烃的这类设备的一个具体实施方案由称为蒸汽裂化器的设施所代表,其中烃可裂化以具体产生乙炔,乙炔又可转化成许多石油化学品,尤其包括乙烯。在这类设备中,耐火陶瓷产品有时必须经受超过2000℃的操作温度,有时甚至还兼有炉内气氛性质的快速改变。
还可能在例如显著更低的温度下,例如甚至在低于1700℃的温度下使烃裂化。但是,在这些温度下,由烃产生乙炔的产率显著降低,为此,如果有可能的话,尽一切努力在高于2,000℃的温度下加工烃。
WO 2009/126357 A1和WO 2010/135073 A2提出在用于烃热处理的设备中使用的基于氧化钇(Y2O3)的耐火陶瓷产品。该同一文献还更详细地描述了用于烃热处理的与物类相关的设备类型。
本发明的目的在于提供用于生产适合在用于烃热处理的设备的馈料器中使用的成形耐火陶瓷产品的组合物。应当可能由所述组合物生产可在处于高于2000℃的应用温度的这类设备中使用的成形耐火陶瓷产品。这类成形耐火陶瓷产品还应该能够经受住在快速演替的还原特征和氧化特征之间起伏的气氛。
本发明的又一目的在于提供用其可能生产能够在处于上述操作条件的这类设备中使用的成形耐火陶瓷产品的方法。
本发明的又一目的在于提供成形耐火陶瓷产品,其可具体由这样的组合物生产且具体用这样的方法生产,且其可用于在上述操作条件下的所述设备中。
在本发明基于提供所述组合物的目的的程度上,为了解决根据本发明的目的,提供用于生产成形耐火陶瓷产品的组合物以便用于烃热处理的设备,所述组合物由以下各物组成:
- 85-99质量%的Y2O3,和
- 1-15质量%的ZrSiO4,
其中以重量%计的值在每种情况下相对于组合物的总质量计算。
本发明的出发点为这样的基本思想,基于氧化钇(Y2O3)的组合物通常可适合提供用于用以烃热处理的成套设备的馈料器的成形耐火陶瓷产品。然而,使用Y2O3作为用于生产成形耐火陶瓷产品的基础原料的缺点在于实践上不可能在资金或技术方面在工业规模上能维持的温度下烧结Y2O3。令人意外的是,在本发明的上下文中,已经揭示,当硅酸锆(ZrSiO4)作为在具有Y2O3基质的组合物中的另一组分使用时,可能生产用于用于在资金和技术方面为大规模工艺所接受的条件下烃热处理的成套设备的成形耐火陶瓷产品,且所述产品满足先前对于这样的产品所阐述的所有要求。
根据现有信息,硅酸锆在基于氧化钇的组合物中的有利作用可归因于以下相关因素:在高于约1640℃的温度下,硅酸盐开始分解成氧化锆(ZrO2)和二氧化硅(SiO2)。然而,在高于硅酸锆的该分解温度1640℃时,由硅酸锆形成的硅酸盐具有高度反应性且与组合物中的氧化钇中的一些钇反应以形成一种或多种硅酸钇。所形成的硅酸钇又形成用于氧化钇的粘合剂相。在硅酸锆分解时形成的至少一些ZrO2进入到所得氧化钇的溶液中。因此,根据本发明的组合物为反应性粘合剂体系,其中所述组合物的组分在约1640℃的温度下开始彼此反应且其中出现中间熔融相,其反应以形成随着反应进行在高温下稳定的相。在陶瓷焙烧期间由该反应形成的耐火陶瓷产品在高于在产品生产期间主导的烧结温度下、尤其甚至在高于2000℃的温度下非常适用。
具体地讲,根据本发明,提供氧化钇(Y2O3)在根据本发明的组合物中以至少85质量%的比例,也就是说,例如还以至少86质量%、87质量%、88质量%、89质量%、90质量%、91质量%、92质量%、93质量%、94质量%、95质量%或96质量%的比例存在。还可提供氧化钇在根据本发明的组合物中以不超过99质量%的比例,也就是说,例如还以不超过98.8质量%、98.6质量%、98.4质量%、98.2质量%、98质量%、97.8质量%、97.6质量%、97.4质量%、97.2质量%或97质量%的比例存在。
除非另外指出,否则在本文件中以质量%给出的值在每种情况下就组合物的总质量而言。
另外,在本文件中给出的关于“粒度”的值是指氧化钇和硅酸锆的相应原料的粒度。
在根据本发明的组合物中氧化钇的粒度优选全部小于4.0mm,或具有小于4.0mm的D90粒度(也就是说,相对于相应组合物的总质量计算的90质量%),也就是说例如还全部小于3.5mm或小于3.15mm。
例如,在每种情况下相对于在根据本发明的组合物中氧化钇的总质量计算,氧化钇在组合物中完全以如下粒度存在或按照如下质量比例以D90粒度存在:
< 4.0mm:100质量%;
< 3.5mm:100质量%;
< 3.15mm:100质量%;
< 2.0mm:至少80、81、82或83质量%。不超过88、87、86或85质量%;
< 1.4mm:至少70、71、72或73质量%。不超过78、77、76、75或74质量%;
< 1.0mm:至少60、61、62、63或64质量%。不超过70、69、68、67、66或65质量%;
< 0.5mm:至少45、46、47、48或49质量%。不超过55、54、53、52、51或50质量%;
< 0.2mm:至少30、31、32、33或34质量%。不超过38、37、36或35质量%;
< 0.1mm:至少20、21、22、23、24、25或26质量%。不超过31、30、29、28或27质量%。
例如,可以提供,在每种情况下相对于在根据本发明的组合物中氧化钇的总质量计算,氧化钇在下文所表示的粒度极限内以相应质量比例存在:
- 2.0mm至< 3.15mm:至少10、11、12、13、14或15质量%。不超过21、20、19、18或17质量%。例如16质量%。
- 1.4mm至< 2.0mm:至少7、8、9或10质量%。不超过15、14、13或12质量%。例如11质量%。
- 1.0mm至< 1.4mm:至少6、7或8质量%。不超过12、11或10质量%。例如9质量%。
- 0.5mm至< 1.0mm:至少10、11、12、13或14质量%。不超过20、19、18、17或16质量%。例如15质量%。
- 0.1mm至< 0.5mm:至少10、11、12、13或14质量%。不超过20、19、18、17或16质量%。例如15质量%。
- 0.1mm至< 0.2mm:至少5、6或7质量%。不超过11、10或9质量%。例如8质量%。
- > 0mm至< 0.1mm:至少20、21、22、23、24或25质量%。不超过31、30、29、28或27质量%。例如26质量%。
ZrSiO4(硅酸锆)在所述组合物中可以至少1质量%的比例,也就是说,例如还以至少1.2质量%、1.4质量%、1.6质量%、1.8质量%、2质量%、2.2质量%、2.4质量%、2.6质量%、2.8质量%或3质量%的比例存在。ZrSiO4在根据本发明的组合物中可以例如不超过15质量%的比例存在,就是说,例如还以不超过14、13、12、11、10、9、8、7、6、5或4质量%的比例存在。
根据本发明,可特别地提供,在所述组合物中ZrSiO4的粒度全部小于1.0mm或具有小于1.0mm的D90粒度,也就是说,全部为例如还小于0.5mm、0.1mm、0.05mm、0.03mm、0.02mm或0.01mm的粒度,或具有例如还小于0.5mm、0.1mm、0.05mm、0.03mm、0.02mm或0.01mm的D90粒度。
根据本发明已经发现,通常存在于用于生产耐火陶瓷产品的组合物中的许多物质对由根据本发明的组合物生产的成形耐火陶瓷产品的耐熔性具有不利作用。具体地讲,这些物质为氧化物TiO2(二氧化钛)、Fe2O3(氧化铁)及碱金属和碱土金属的氧化物,特别是Na2O、K2O、CaO、MgO和BaO。
根据本发明,因此可提供,所述组合物包含以不超过以下最大比例的量的这些氧化物中的至少一种或这些氧化物的总和:
- TiO2 ≤ 0.15质量%;
- Fe2O3 ≤ 0.15质量%;
- Na2O + K2O ≤ 0.15质量%;
- CaO + MgO + BaO ≤ 0.20质量%。
氧化铝(Al2O3)还可对根据本发明的组合物的烧结有不合需要的作用,但少量的该物质在所述组合物中是可容许的。根据本发明可提供,所述组合物含有比例小于3质量%的Al2O3,也就是说,例如还小于2.5质量%、2质量%、1.5质量%、1质量%、0.5质量%或0.1质量%的Al2O3。
用于用以烃热处理的设备的具有特别优良的性质的成形耐火陶瓷产品随后可由根据本发明的组合物制备,特别是如果这类组合物几乎不含除氧化钇和硅酸锆以外的组分或仅含非常少量的所述组分。根据一个实施方案,提供根据本发明的组合物仅包含总量小于5质量%的除氧化钇和硅酸锆以外的组分,也就是说,例如还小于4质量%、3质量%、2质量%、1质量%、0.8质量%、0.6质量%、0.5质量%、0.4质量%、0.3质量%、0.2质量%或0.1质量%的所述组分。如果根据本发明的组合物包含除氧化钇和硅酸锆之外的其他组分,则这些组分可特别地经由天然杂质引入所述组合物中。
为了确保在所述组合物中存在尽可能最少量的除氧化钇和硅酸锆以外的组分,优选提供氧化钇和硅酸锆各自作为非常纯的形式的原料存在于所述组合物中。
本发明的主题还为由根据本发明的组合物生产成形耐火陶瓷产品的方法,其包括以下步骤:
- 提供根据本发明的组合物;
- 混合所述组合物与粘合剂;
- 将与粘合剂混合的所述组合物模塑成成形体;
- 焙烧所述成形体以形成成形耐火陶瓷产品。
进行根据本发明的组合物与粘合剂的混合以使所述组合物具有可模塑的坚实度(consistency)。混合所述组合物与粘合剂使得所述组合物能够模塑成具有足够固有稳定性从而其能够接着经历进一步加工而不失去其形状的成形体(生坯)。
通常,根据本发明的组合物可与从现有技术对于基于用于耐火材料的氧化物的组合物已知的任何粘合剂混合。根据本发明的组合物优选与有机粘合剂混合,例如以下粘合剂中的至少一种:糊精、水果酸、糖或聚乙烯醇。
所述组合物可与例如以至少0.2质量%的量、也就是说例如还以至少0.3质量%、0.4质量%或0.5质量%的量的粘合剂混合。所述组合物可与以不超过例如2质量%的量,也就是说例如还以不超过1.5质量%、1质量%、0.8质量%或0.6质量%的量的粘合剂混合。在每种情况下,关于粘合剂的质量的值相对于没有粘合剂的组合物的总质量计算,也就是说相对于100质量%的没有粘合剂的组合物计算。
在耐火技术中,基于氧化物的组合物常与磷酸盐粘合剂混合。然而,在本发明的上下文中已经发现,磷或含磷化合物可对根据本发明的烧结的成形耐火陶瓷产品具有不利作用。因此,可以提供不使用以磷酸盐粘合剂形式的粘合剂。还可以提供所述组合物含有以不超过0.1质量%的量,就是说例如还以不超过0.05质量%或0.01质量%的量的磷(以P2O5形式计算)。
与粘合剂混合的组合物可在其例如在桨叶式混合器中成型之前混合。
使与粘合剂混合的组合物成型以形成成形体(生坯)优选通过压制进行。
所述成形体可在焙烧之前例如在110-250℃的温度下干燥。
焙烧所述成形体以生产成形耐火陶瓷产品是一种陶瓷焙烧方法,其中所述组合物的组分彼此烧结在一起以生产耐火陶瓷产品。通过焙烧成形体,获得相应烧结的成形耐火陶瓷产品。
所述组合物或由所述组合物生产的成形体例如在超过1640℃的温度下且优选在至少1700℃或1750℃的温度下且例如在不超过1850℃或1800℃的温度下焙烧。
焙烧例如进行例如6-8小时的时间。
本发明的又一目的为具体通过根据本发明的方法生产的成形耐火陶瓷产品。
如先前所解释,根据本发明的组合物为反应性粘合剂体系,其中所述组分在陶瓷焙烧期间彼此反应以形成先前描述的反应产物。因此,本发明的主题还为包含以下相的成形耐火陶瓷产品:
- Y2O3;
- Y2O3-ZrO2固溶体;和
- 硅酸钇。
先前描述的相是已经由根据本发明的组合物生产的成形耐火陶瓷产品的特征。所述产品的主相为氧化钇(Y2O3),其与以硅酸钇形式的粘合剂相一起烧结。还存在Y2O3-ZrO2固溶体。
根据本发明的成形耐火陶瓷产品还可包含以下相中的至少一个:ZrO2(作为ZrSiO4分解的产物)和硅酸锆(尚未分解的少量残留)。
如果硅酸钇存在于根据本发明的成形耐火陶瓷产品中,则这些可为以下硅酸钇中的一种或多种:Y2SiO5 (SiO2 . Y2O3)、Y2Si2O7 (2SiO2 . Y2O3)或Y4Si3O12 (3SiO2 . 2Y2O3)。
在每种情况下相对于根据本发明的产品的总质量计算,根据本发明的产品可包含例如以至少76.5质量%的比例,也就是说,例如以至少78、80、82、84、86、88、90、92、94或95质量%的比例的相Y2O3和Y2O3-ZrO2固溶体。例如,在每种情况下,相对于根据本发明的产品的总质量计算,在根据本发明的产品中的Y2O3和Y2O3-ZrO2固溶体的总质量可为不超过98.5质量%的量,也就是说,例如还为不超过98质量%、97.5质量%、97质量%、96.5质量%或96质量%的量。
在每种情况下,相对于根据本发明的产品的总质量计算,在根据本发明的产品中硅酸钇的质量可例如为至少1.5质量%,也就是说,例如还为至少2质量%、2.5质量%、3质量%、3.5质量%或4质量%。在每种情况下,相对于根据本发明的产品的总质量计算,在根据本发明的产品中硅酸钇的质量可例如以不超过23.5质量%的量,就是说例如还以不超过20、18、16、14、12、10、6、7、6或5质量%的量。
根据本发明可提供,在每种情况下,相对于根据本发明的产品的总质量计算,存在于根据本发明的产品中的除Y2O3、Y2O3-ZrO2固溶体、硅酸钇、ZrO2和ZrSiO4以外的相的总质量小于5质量%,也就是说,例如还小于4质量%、3质量%、2质量%、1质量%、0.8质量%、0.6质量%或0.5质量%。
根据本发明的成形耐火陶瓷产品在优良耐火性质方面是显著的。根据本发明的产品可例如表现出以下物理性质中的至少一种:
- 低温耐压强度[MPa]: ≥ 40、≥ 45、≥ 50、≥ 55且例如≤ 100、≤ 90、≤ 80、≤ 70、≤ 60;
- 气体渗透率[nPm]: ≥ 2.8、≥ 2.9、≥ 3且例如≤ 3.5、≤ 3.4、≤ 3.3;
- 堆密度[g/cm3]: ≥ 3.9、≥ 3.91、≥ 3.92且例如≤ 4.02、≤ 4.01、≤ 4.0、≤ 3.99、≤ 3.98、≤ 3.97、≤ 3.96、≤ 3.95、≤ 3.94;
- 开口孔隙率[体积%]: ≥ 14、≥ 15、≥ 16、≥ 17且例如≤ 24、≤ 23、≤ 22、≤ 21、≤ 20、≤ 19;
- 荷重耐熔度T0[℃]: ≥ 1600、≥ 1620、≥ 1640、≥ 1660、≥ 1680;
- 荷重耐熔度T0.5[℃]: ≥ 1680、≥ 1685、≥ 1690、≥ 1695、≥ 1700;
- 在2000℃下的长度永久改变[%]: ≤ -0.5、≤ -0.6、≤ -0.7、≤ -0.8、≤ -0.9、≤ -1.0。
低温耐压强度根据DIN EN 993-5:1998测定。
气体渗透率根据DIN EN 993-4:1995测定。
堆密度根据DIN EN 993-1:1995测定。
开口孔隙率根据DIN EN 993-1:1995测定。
荷重耐熔度根据DIN EN 1893:2008测定。
长度永久变形根据DIN EN 993-10:1998测定。
根据本发明的产品可在高温(例如> 1800℃)下表现出气氛条件(例如,还原/氧化性气氛)的强烈变化的设备中使用。具体地讲,根据本发明的产品可用于在所述设备中的馈料器,其中所述产品暴露于高于2000℃的操作温度。
另外,本发明的产品可用于石油化学设备中,特别是分别用于裂化工艺或石油化学裂化器中。
通常,本发明的产品可用于高温工艺中。例如,本发明的产品可用于其中它们暴露于高于2000℃的温度的工艺中。
根据一个实施方案,本发明的产品可用于设备中且用于用以生产碳黑的方法中,例如用于灯黑、气黑、炉黑或乙炔黑方法中。
根据另一实施方案,本发明的产品可作为用于焙烧喷嘴,即燃烧器喷嘴的材料使用。
根据一个实施方案,根据本发明的组合物包含以如下质量比例的以下组分:
Y2O3:97质量%;
ZrSiO4:3质量%。
所述Y2O3具有全部小于3.15mm的粒度且所述ZrSiO4具有全部小于0.01mm的粒度。
根据本发明方法的一个实施方案,将根据所述实施方案的组合物与相对于100质量%的没有粘合剂的组合物计算0.5质量%的粘合剂混合,所述粘合剂以糊精形式,且随后将混合物在桨叶式混合器中混合。随后将组合物和粘合剂的混合物模塑以通过压制形成成形体,随后在150℃下干燥且最后在1800℃下焙烧7小时的时间以生产成形耐火陶瓷产品。
在每种情况下相对于所述产品的总质量计算,以此方式生产的烧结产品包含以下重量比例的以下相:
Y2O3和Y2O3-ZrO2固溶体的总量:95.34%质量;
硅酸钇:4.66%质量。
通过所述实施例的方法生产的产品的物理性质如下:
- 低温耐压强度[MPa]:58.8;
- 气体渗透率[nPm]:3.15;
- 堆密度[g/cm3]:3.98;
- 开口孔隙率[体积%.]:20.4;
- 在载重T0下的耐熔度[℃]:1688;
- 在载重T0.5下的耐熔度[℃]:大于1699;
- 在2000℃下的长度永久改变[%]:-1.04。
Claims (8)
1.生产成形耐火陶瓷产品的组合物,其包含:
85-99%质量的Y2O3;和
1-15质量%的ZrSiO4;
在每种情况下相对于所述组合物的总质量计算。
2.根据权利要求1的组合物,其中存在的Y2O3具有小于4.0mm的粒度。
3.根据前述权利要求中任一项的组合物,其中存在的ZrSiO4具有小于1.0mm的粒度。
4.根据权利要求1或2的组合物,其包含在每种情况下以所指出的最大比例的以下氧化物中的至少一种或氧化物的总和:
TiO2 ≤ 0.15质量%;
Fe2O3 ≤ 0.15质量%;
Na2O + K2O ≤ 0.15质量%;
CaO + MgO + BaO ≤ 0.20质量%;
在每种情况下相对于所述组合物的总质量计算。
5.由根据前述权利要求中任一项的组合物生产成形耐火陶瓷产品的方法,所述方法包括以下步骤:
提供根据前述权利要求中任一项的组合物;
混合所述组合物与粘合剂;
将与粘合剂混合的所述组合物模塑成成形体;
焙烧所述成形体以形成成形耐火陶瓷产品。
6.由根据权利要求5的方法提供的成形耐火陶瓷产品。
7.根据权利要求6的成形耐火陶瓷产品,其包含以下相:
Y2O3;
Y2O3-ZrO2固溶体;和
硅酸钇。
8.根据权利要求6的成形耐火陶瓷产品,其具有以下物理性质中的至少一种:
- 低温耐压强度 ≥ 40 MPa;
- 气体渗透率 ≤ 3.5 nPm;
- 堆密度 ≥ 3.90 g/cm3;
- 开口孔隙率 ≤ 24体积%;
- 荷重耐熔度T0 ≥ 1600℃;
- 荷重耐熔度T0.5 ≥ 1680℃;
- 在2000℃下的长度永久改变 ≤ -0.5%。
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PCT/EP2015/050989 WO2015149956A1 (en) | 2014-04-03 | 2015-01-20 | Composition for producing a shaped refractory ceramic product, a method for producing a shaped refractory ceramic product, and a shaped refractory ceramic product |
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CN101628812A (zh) * | 2008-07-14 | 2010-01-20 | 东北大学 | 一种制备致密氧化钇陶瓷的方法 |
CN102803179A (zh) * | 2009-06-12 | 2012-11-28 | 特莱巴赫工业有限公司 | 氧化钇基浆料组合物 |
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US7976797B2 (en) | 2008-04-08 | 2011-07-12 | Exxonmobil Chemical Patents Inc. | Advanced materials for regenerative pyrolysis reactors, methods, and reactors using the same |
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