CN113603490A - 高熵陶瓷惰性基弥散燃料芯块及其制备方法 - Google Patents

高熵陶瓷惰性基弥散燃料芯块及其制备方法 Download PDF

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CN113603490A
CN113603490A CN202110831853.XA CN202110831853A CN113603490A CN 113603490 A CN113603490 A CN 113603490A CN 202110831853 A CN202110831853 A CN 202110831853A CN 113603490 A CN113603490 A CN 113603490A
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powder
core
metal
raw material
entropy ceramic
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CN113603490B (zh
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薛佳祥
吴利翔
张显生
任啟森
廖业宏
张永栋
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China General Nuclear Power Corp
China Nuclear Power Technology Research Institute Co Ltd
CGN Power Co Ltd
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China General Nuclear Power Corp
China Nuclear Power Technology Research Institute Co Ltd
CGN Power Co Ltd
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Abstract

本发明公开了一种高熵陶瓷惰性基弥散燃料芯块及其制备方法,制备方法包括:S1、将原料粉体分别制成浆料和混合粉体;S2、将浆料喷涂在滚动的燃料颗粒表面,烘干后形成粘附在燃料颗粒表面的包覆层;S3、制备核心素坯和核壳素坯;S4、将核心素坯装入核壳素坯内,热处理,得到陶瓷坯体;S5、固熔烧结,形成致密化的高熵陶瓷惰性基弥散燃料芯块。本发明通过原位反应‑固熔烧结两步法制备获得高熵陶瓷惰性基弥散燃料芯块,实现燃料芯块的热导率高、肿胀低、易后处理和适合工业化生产等特点;提高核反应堆包壳破损情况下的核燃料包容性,阻止核燃料的泄漏,提高核电安全性;改善核燃料的耐高温性能,推动核燃料在高温堆的应用。

Description

高熵陶瓷惰性基弥散燃料芯块及其制备方法
技术领域
本发明涉及核燃料技术领域,尤其涉及一种高熵陶瓷惰性基弥散燃料芯块及其制备方法。
背景技术
随着工业的发展,对能源的需求量也越来越大,核能作为一种清洁能源备受各行各业的青睐。随着对核能利用率的快速增长,随之而来的安全问题也不容忽视。其中,堆芯燃料在极端事故环境下不发生熔化或不泄漏是核反应堆安全的重要保障。目前主要采用包壳来保证核燃料不泄漏,但包壳仍存在破损的可能性。美国提出的全陶瓷包覆燃料(FCM),通过采用SiC惰性基体,使得安全性得到极大地提高。然而SiC惰性基体在辐照后热导率低于10W/m·K,导致燃料中心温度极易升高,同时FCM的SiC惰性基体会受到裂变产物Pd、Ag和Cs等的侵蚀,安全许用温度在1600℃以下。
碳化锆(ZrC)作为超高温陶瓷,具有优异的高温稳定性能(熔点为3530℃且不发生高温相变),因其中子吸收截面小、耐核裂变产物腐蚀、辐照后热导率高、耐铅铋和熔盐腐蚀,作为新型反应堆弥散燃料的惰性基体具有大的前景。但是,ZrC的烧结温度高达2200℃左右,且高温烧结又易造成材料显微组织粗化严重。并且,ZrC烧结过程中通常需要添加烧结助剂,烧结助剂的使用不仅降低其高温性能,还会降低其耐腐蚀、抗辐照等综合性能。
发明内容
本发明要解决的技术问题在于,提供一种烧结温度低、热导率高、肿胀率低的高熵陶瓷惰性基弥散燃料芯块及其制备方法。
本发明解决其技术问题所采用的技术方案是:提供一种高熵陶瓷惰性基弥散燃料芯块,包括以下步骤:
S1、将原料粉体分别制成浆料和混合粉体;
所述原料粉体包括五种或五种以上的金属粉体、金属氧化物粉体或金属氢化物粉体;
S2、将所述浆料喷涂在滚动的燃料颗粒表面,烘干后形成粘附在燃料颗粒表面的包覆层;
S3、将一部分所述混合粉体与带有包覆层的燃料颗粒按比例混合后,压制形成柱状的核心素坯;将另一部分所述混合粉体压制形成筒状的核壳素坯;
S4、将所述核心素坯装入所述核壳素坯内,在第一设定气氛下进行热处理,使所述核心素坯和核壳素坯中的原料粉体进行原位反应,得到陶瓷坯体;
S5、将所述陶瓷坯体在第二设定气氛下进行固熔烧结,形成致密化的高熵陶瓷惰性基弥散燃料芯块。
优选地,所述金属粉体、金属氧化物粉体和金属氢化物粉体中的金属包括Zr、Ti、Nb、Ta、V、Cr、Mo和W中至少五种;所述原料粉体的粒径为10nm~200μm。
优选地,步骤S1包括:
S1.1、将原料粉体与分散剂、有机溶剂进行混合形成浆料;
S1.2、将部分所述混合浆料通过干燥处理形成混合粉体;或者,将原料粉体与分散剂混合形成混合粉体。
优选地,在所述浆料中,所述有机溶剂与所述原料粉体的质量比例为1:1~3:1;所述分散剂占所述原料粉体的质量百分比为0.5%~4%。
优选地,所述分散剂为聚乙烯亚胺、四甲基氢氧化铵中至少一种;所述有机溶剂为无水乙醇、丙酮中至少一种。
优选地,步骤S2中,所述燃料颗粒包括TRISO颗粒、UO2、UC、UC2、UN、UCN、UCO、U3Si2、U合金、PuO2、PuC、PuN、Pu合金中至少一种;
所述TRISO颗粒的核心包括UO2、UC、UC2、UN、UCN、UCO、U3Si2、U合金中至少一种。
优选地,步骤S2中,所述燃料颗粒在滚动的同时加热到50℃~100℃;采用气压喷雾装置将所述浆料喷涂在燃料颗粒表面。
优选地,步骤S3中,所述核心素坯在10MPa~100MPa的压力下成型;所述核壳素坯在30MPa~400MPa的压力下成型。
优选地,步骤S4中,所述热处理的温度为800℃-1200℃;
步骤S5中,固熔烧结的温度为1300℃-1550℃。
优选地,在所述原料粉体为五种或五种以上的金属粉体、五种或五种以上的金属氧化物粉体或五种或五种以上的金属氢化物粉体的混合粉体时,步骤S4中,所述第一设定气氛为氮气;
在氮气气氛下,各金属粉体、金属氧化物或者金属氢化物分别与氮气进行原位反应,生成氮化物陶瓷;
步骤S5中,所述第二设定气氛为真空、氩气、氦气或氮气。
优选地,所述原料粉体的各粉体之间的摩尔比为1:1。
优选地,步骤S1中,所述原料粉体还包括C粉或Si粉;
步骤S4中,所述第一设定气氛为真空、氩气、氦气或氮气;
在第一设定气氛下,各金属粉体、金属氧化物或者金属氢化物分别与C或Si进行原位反应,生成碳化物、氮化物、碳氮化物或硅化物陶瓷;
步骤S5中,所述第二设定气氛为真空、氩气、氦气或氮气。
优选地,所述原料粉体中,各金属粉体之间的摩尔比为1:1,各金属氧化物粉体之间的摩尔比1:1,各金属氢化物粉体之间的摩尔比1:1;
所述C粉与各金属粉体或各金属氢化物粉体之间的摩尔比为1:1,所述C粉与各金属氧化物粉体之间的摩尔比为3:1;
所述Si粉与各金属粉体、各金属氧化物粉体或各金属氢化物粉体之间的摩尔比为1:1。
本发明还提供一种高熵陶瓷惰性基弥散燃料芯块,采用以上任一项所述的制备方法制得。
本发明的有益效果:通过原位反应-固熔烧结两步法制备获得高熵陶瓷惰性基弥散燃料芯块,以高熵陶瓷惰性基作为燃料芯块的基体,相比于SiC惰性基的燃料芯块具有更高的耐高温、耐腐蚀及抗辐照性能,实现燃料芯块的热导率高、肿胀低、易后处理和适合工业化生产等特点;提高核反应堆包壳破损情况下的核燃料包容性,阻止核燃料的泄漏,提高核电安全性;改善核燃料的耐高温性能,推动核燃料在高温堆的应用。
本发明的高熵陶瓷惰性基弥散燃料芯块适用于轻水堆、气体冷却反应堆(高温气体反应堆或超高温气体反应堆)、熔融金属冷却反应堆或快中子增殖反应堆等核反应堆中燃料芯块。
附图说明
下面将结合附图及实施例对本发明作进一步说明,附图中:
图1是本发明的高熵陶瓷惰性基弥散燃料芯块的剖面结构示意图。
具体实施方式
本发明的高熵陶瓷惰性基弥散燃料芯块的制备方法,可包括以下步骤:
S1、将原料粉体分别制成浆料和混合粉体。
该步骤S1进一步可包括:
S1.1、将原料粉体与分散剂、有机溶剂进行混合形成浆料。
具体地,将原料粉体、分散剂及有机溶剂在辊式球磨机上进行球磨混合,以50r/min~200r/min的转速球磨1h~10h,采用的磨球为氮化硅,球料比(磨球和混料的质量比例)为1:1~4:1。
在浆料中,有机溶剂与原料粉体的质量比例为1:1~3:1。
分散剂为聚乙烯亚胺、四甲基氢氧化铵中至少一种。有机溶剂为无水乙醇、丙酮中至少一种。
S1.2、将部分混合浆料通过干燥处理形成混合粉体;或者,将原料粉体与分散剂混合形成混合粉体。
在浆料以及混合粉体中,分散剂占原料粉体的质量百分比均为0.5%~4%。
其中,原料粉体包括五种或五种以上的金属粉体、金属氧化物粉体或金属氢化物粉体;或者,原料粉体包括C粉(碳粉)或Si粉(硅粉)、以及五种或五种以上的金属粉体、金属氧化物粉体或金属氢化物粉体。原料粉体的粒径为10nm~200μm。
原料粉体中,金属粉体、金属氧化物粉体和金属氢化物粉体中的金属包括Zr、Ti、Nb、Ta、V、Cr、Mo和W中至少五种。因此,当原料粉体包括至少五种金属粉体时,即包括Zr粉、Ti粉、Nb粉、Ta粉、V粉、Cr粉、Mo粉和W粉中至少五种,各金属粉体之间的摩尔比为1:1;当原料粉体包括至少五种金属氧化物粉体时,即包括至少五种前述金属对应的氧化物,各金属氧化物粉体之间的摩尔比为1:1;当原料粉体包括至少五种金属氢化物粉体时,即包括至少五种前述金属对应的的氢化物,各金属氢化物粉体之间的摩尔比为1:1。
当原料粉体还包括C粉时,C粉与各金属粉体或各金属氢化物粉体之间的摩尔比为1:1,C粉与各金属氧化物粉体之间的摩尔比为3:1。
当原料粉体还包括Si粉时,Si粉与各金属粉体、各金属氧化物粉体或各金属氢化物粉体之间的摩尔比为1:1。
S2、采用气压喷雾装置将浆料喷涂在滚动的燃料颗粒表面,烘干后形成粘附在燃料颗粒表面的包覆层。
燃料颗粒在滚动的同时加热到50℃~100℃;由于加热作用,浆料中的有机溶剂挥发去除。
其中,燃料颗粒可包括TRISO颗粒、UO2、UC、UC2、UN、UCN、UCO、U3Si2、U合金、PuO2、PuC、PuN、Pu合金中至少一种。TRISO颗粒的核心包括UO2、UC、UC2、UN、UCN、UCO、U3Si2、U合金中至少一种。
S3、将一部分混合粉体与带有包覆层的燃料颗粒按比例混合后,压制形成柱状的核心素坯;将另一部分混合粉体压制形成筒状的核壳素坯。
核心素坯在10MPa~100MPa的压力下成型。核心素坯的直径可为6mm~8mm,高8mm~24mm。
核壳素坯在30MPa~400MPa的压力下成型。核壳素坯的内径可为6.2mm~8.2mm,外径可为8.5mm~10mm,高可为8mm~24mm。
S4、将核心素坯装入核壳素坯内,在第一设定气氛下进行热处理,使核心素坯和核壳素坯中的原料粉体进行原位反应,得到陶瓷坯体。
热处理的温度为800℃-1200℃,优选1000℃-1200℃。在热处理温度达到所需温度后,保温0.5h-10h,优选0.5h-2h。
S5、将陶瓷坯体在第二设定气氛下进行固熔烧结,形成致密化的高熵陶瓷惰性基弥散燃料芯块。
该固熔烧结可在无压下进行。固熔烧结的温度为1300℃-1550℃,优选1400℃-1550℃。在固熔烧结温度达到所需温度后,保温0.5h-10h,优选0.5h-2h。
作为选择,当原料粉体为五种或五种以上的金属粉体、五种或五种以上的金属氧化物粉体或五种或五种以上的金属氢化物粉体的混合粉体时,在步骤S4中,第一设定气氛为氮气。在氮气气氛下,各金属粉体、金属氧化物或者金属氢化物分别与氮气进行原位反应,生成氮化物陶瓷。
金属粉体(M)与氮气(N2)进行原位反应生成氮化物的反应式如下:
2M+xN2=2MNX
金属氢化物粉体(MHX)与氮气(N2)进行原位反应生成氮化物的反应式如下:
3MHX+(x/2+3y/2)N2=3MNy+xNH3
上述各反应式中,x为1-4,通常为1或2;y为1-2,通常为1。
在步骤S5的固熔烧结中,第二设定气氛为真空、氩气、氦气或氮气,在该第二设定气氛下,各氮化物陶瓷固熔形成一体。
当原料粉体包括五种或五种以上的金属粉体、金属氧化物粉体或金属氢化物粉体,还包括C粉或Si粉时,在步骤S4中,第一设定气氛为真空、氩气、氦气或氮气。在第一设定气氛下,各金属粉体、金属氧化物或者金属氢化物分别与C或Si进行原位反应,生成碳化物、氮化物、碳氮化物或硅化物陶瓷。
金属粉体(M)与C进行原位反应生成碳化物的反应式如下:
M+xC=MCX
金属氧化物粉体(MOX)与C进行原位反应生成碳化物的反应式如下:
MOX+(x+y)C=MCy+xCO
金属氢化物粉体(MHX)与C进行原位反应生成碳化物的反应式如下:
2MHX+2yC=2MCy+xH2
金属氢化物粉体(MHX)与C进行原位反应生成碳氮化物的反应式如下:
MOX+(x+y/2)C+(x/2+y/4)N2=M(C0.5N0.5)y+xCO
金属粉体(M)与Si进行原位反应生成硅化物的反应式如下:
2M+xSi=2MSiX
金属氢化物粉体(MHX)与Si进行原位反应生成硅化物的反应式如下:
2MHX+2ySi=2MSiy+xH2
上述各反应式中,x为1-4,通常为1或2;y为1-2,通常为1。
经原位反应后,在步骤S5的固熔烧结中,第二设定气氛为真空、氩气、氦气或氮气。
上述的制备方法中,通过原料粉体中进行的原位反应,减小高熵粉体杂质含量,提高高熵陶瓷惰性基体的纯度,同时降低制备成本。
上述制得的致密化的高熵陶瓷惰性基弥散燃料芯块,其致密度高于95%,杂质氧元素的含量低于0.1wt%。
参考图1,本发明的制备方法制得的高熵陶瓷惰性基弥散燃料芯块,包括柱状的燃料区10以及筒状的无燃料区20。燃料区10设置在无燃料区20且两者紧密结合。其中,燃料区10由核心素坯形成,无燃料区20由核壳素坯形成。燃料区10包括高熵陶瓷惰性基体11以及弥散在高熵陶瓷惰性基体11中的燃料颗粒12。高熵陶瓷惰性基体11及无燃料区20均由原料粉体经原位反应和固熔烧结后形成。
高熵陶瓷惰性基体11相比于SiC惰性基具有更高的耐高温、耐腐蚀、抗辐照性能,能够提高核燃料高温稳定性和辐照后热导率,降低堆芯熔化风险,提高安全性。随着辐照剂量增加和温度升高,燃料的高熵陶瓷惰性基体11肿胀率能够保持在0.3%以下。在乏燃料后处理时,可以采用强酸或氟盐进行湿法或干法分离。
下面通过具体实施例对本发明作进一步说明。
实施例1
以ZrO2、TiO2、NbO2、TaO2、MoO2和C为原料粉体,以上粉体纯度为99.9%,粒径为20nm,以上各金属氧化物粉体之间的摩尔比为1:1,各金属氧化物粉体与C之间的摩尔比为1:3;以聚乙烯亚胺为分散剂,含量占以上原料粉体的2wt%,以无水乙醇为有机溶剂,有机溶剂质量和以上原料粉体和分散剂综合的比例为2:1。按照以上比例在辊式球磨中进行混合,磨球为氮化硅,转数为100r/min,球磨时间为12h,球磨后制备得到浆料,将其中一部分浆料通过旋转蒸发并且干燥制备得到混合粉体。
采用装载UO2铀燃料的TRISO颗粒作为燃料颗粒,TRISO颗粒从内而外依次为疏松热解炭层、内致密热解炭层、碳化硅层和外致密热解炭层,将TRISO颗粒在滚动状态下加热到90℃,通过喷雾沉积将以上浆料在TRISO颗粒进行“穿衣”,对“穿衣”后的TRISO颗粒在90℃下去除有机溶剂,得到“穿衣”后的TRISO颗粒,随后将“穿衣”后的TRISO颗粒与前述制备的混合粉体以40wt%的比例含量进行干压,机械加压压力为100MPa,压制得到直径为8mm、高8mm的圆柱状核芯素坯。
再将不含燃料颗粒的混合粉体在80MPa压力下压制成内径8.2mm、外径10mm、高8mm的核壳素坯,将以上核心素坯装入核壳素坯中,在无压炉中以20℃/min升温至1000℃,保温2h后升温至1500℃,保温1h,烧结气氛为氩气。通过以上操作,制备得到高熵陶瓷惰性基弥散燃料芯块((Zr0.2Ti0.2Nb0.2Ta0.2Mo0.2)C),其高熵陶瓷惰性基体致密度达到96%。
得到的(Zr0.2Ti0.2Nb0.2Ta0.2Mo0.2)C高熵陶瓷惰性基弥散燃料芯块中,TRISO颗粒弥散分布在惰性基核燃料核芯,边缘无燃料区可进一步防止核燃料因为TRISO颗粒破损造成的泄漏。
将上述制得的燃料芯块装入包壳管内部完成组装,组装密封后的包壳可用于轻水堆、高温气冷堆、熔岩堆等堆型。
实施例2
以Zr、Cr、Nb、Ta、Mo和C为原料粉体,以上粉体纯度为99.99%,粒径为100nm;以上各金属粉体之间的摩尔比为1:1,各金属粉体与C之间的摩尔比为1:1。按照实施例1方法分别制备核壳素坯和核芯素坯,核芯素坯在50MPa压力下成型,尺寸为直径7mm、高度10mm;核壳素坯在200MPa压力下压制成型,内径为7.2mm、外径为9mm、高度10mm。将以上核芯素坯装入核壳素坯后在无压炉中进行烧结,以15℃/min升温速率加热到1200℃,保温1.5h后再升温至1550℃,保温2h,烧结气氛为真空,制备得到高熵陶瓷惰性基弥散燃料芯块((Zr0.2Cr0.2Nb0.2Ta0.2Mo0.2)C),其高熵陶瓷惰性基体致密度为98%。
实施例3
以ZrO2、CrO2、NbO2、VO2、TaO2、MoO2和C为原料粉体,以上粉体纯度为99.99%,粒径为100nm;以上各金属氧化物粉体之间的摩尔比为1:1,各金属氧化物粉体与C之间的摩尔比为1:3。
按照实施例1方法分别制备核壳素坯和核芯素坯,核芯素坯在100MPa压力下成型,尺寸为直径8mm、高度20mm;核壳素坯在400MPa压力下压制成型,内径为8.2mm、外径为10mm、高度20mm。将以上核芯素坯装入核壳素坯后在无压炉中进行烧结,以5℃/min升温速率加热到1100℃,保温2h后再升温至1450℃,保温4h,烧结气氛为氮气,制备得到高熵陶瓷惰性基弥散燃料芯块((Zr0.16Cr0.16Nb0.16Ta0.16Mo0.16)C0.5N0.5),其高熵陶瓷惰性基体致密度为97%。
实施例4
以ZrH2、TiH2、NbH2、VH2、TaH2、MoH2和Si为原料粉体,以上粉体纯度为99.99%,粒径为50nm;以上各金属氢化物粉体之间的摩尔比为1:1,各金属氢化物粉体与Si之间的摩尔比为1:1。
按照实施例1方法分别制备核壳素坯和核芯素坯,核芯素坯在10MPa压力下成型,尺寸为直径8mm、高度24mm;核壳素坯在300MPa压力下压制成型,内径为8.2mm、外径为10mm、高度24mm。将以上核芯素坯装入核壳素坯后在无压炉中进行烧结,以10℃/min升温速率加热到900℃,保温4h后再升温至1500℃,保温1h,烧结气氛为真空,制备得到高熵陶瓷惰性基弥散燃料芯块((Zr0.2Ti0.2Nb0.2Ta0.2Mo0.2)Si),其高熵陶瓷惰性基体致密度为98%。
实施例5
以Zr、Cr、Nb、Ta、V和Si为原料粉体,以上粉体纯度为99.99%,粒径为200μm;以上各金属粉体之间的摩尔比为1:1,各金属粉体与Si之间的摩尔比为1:1。
按照实施例1方法分别制备核壳素坯和核芯素坯,核芯素坯在100MPa压力下成型,尺寸为直径6mm、高度8mm;核壳素坯在400MPa压力下压制成型,内径为6.2mm、外径为8mm、高度8mm。将以上核芯素坯装入核壳素坯后在无压炉中进行烧结,以10℃/min升温速率加热到1000℃,保温3h后再升温至1550℃,保温5h,烧结气氛为真空,制备得到高熵陶瓷惰性基弥散燃料芯块((Zr0.2Cr0.2Nb0.2Ta0.2V0.2)Si),其高熵陶瓷惰性基体致密度为96%。
以上所述仅为本发明的实施例,并非因此限制本发明的专利范围,凡是利用本发明说明书及附图内容所作的等效结构或等效流程变换,或直接或间接运用在其他相关的技术领域,均同理包括在本发明的专利保护范围内。

Claims (14)

1.一种高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,包括以下步骤:
S1、将原料粉体分别制成浆料和混合粉体;
所述原料粉体包括五种或五种以上的金属粉体、金属氧化物粉体或金属氢化物粉体;
S2、将所述浆料喷涂在滚动的燃料颗粒表面,烘干后形成粘附在燃料颗粒表面的包覆层;
S3、将一部分所述混合粉体与带有包覆层的燃料颗粒按比例混合后,压制形成柱状的核心素坯;将另一部分所述混合粉体压制形成筒状的核壳素坯;
S4、将所述核心素坯装入所述核壳素坯内,在第一设定气氛下进行热处理,使所述核心素坯和核壳素坯中的原料粉体进行原位反应,得到陶瓷坯体;
S5、将所述陶瓷坯体在第二设定气氛下进行固熔烧结,形成致密化的高熵陶瓷惰性基弥散燃料芯块。
2.根据权利要求1所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,所述金属粉体、金属氧化物粉体和金属氢化物粉体中的金属包括Zr、Ti、Nb、Ta、V、Cr、Mo和W中至少五种;所述原料粉体的粒径为10nm~200μm。
3.根据权利要求1所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,步骤S1包括:
S1.1、将原料粉体与分散剂、有机溶剂进行混合形成浆料;
S1.2、将部分所述混合浆料通过干燥处理形成混合粉体;或者,将原料粉体与分散剂混合形成混合粉体。
4.根据权利要求3所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,在所述浆料中,所述有机溶剂与所述原料粉体的质量比例为1:1~3:1;所述分散剂占所述原料粉体的质量百分比为0.5%~4%。
5.根据权利要求3所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,所述分散剂为聚乙烯亚胺、四甲基氢氧化铵中至少一种;所述有机溶剂为无水乙醇、丙酮中至少一种。
6.根据权利要求1所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,步骤S2中,所述燃料颗粒包括TRISO颗粒、UO2、UC、UC2、UN、UCN、UCO、U3Si2、U合金、PuO2、PuC、PuN、Pu合金中至少一种;
所述TRISO颗粒的核心包括UO2、UC、UC2、UN、UCN、UCO、U3Si2、U合金中至少一种。
7.根据权利要求1所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,步骤S2中,所述燃料颗粒在滚动的同时加热到50℃~100℃;采用气压喷雾装置将所述浆料喷涂在燃料颗粒表面。
8.根据权利要求1所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,步骤S3中,所述核心素坯在10MPa~100MPa的压力下成型;所述核壳素坯在30MPa~400MPa的压力下成型。
9.根据权利要求1所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,步骤S4中,所述热处理的温度为800℃-1200℃;
步骤S5中,固熔烧结的温度为1300℃-1550℃。
10.根据权利要求1-9任一项所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,在所述原料粉体为五种或五种以上的金属粉体、五种或五种以上的金属氧化物粉体或五种或五种以上的金属氢化物粉体的混合粉体时,步骤S4中,所述第一设定气氛为氮气;
在氮气气氛下,各金属粉体、金属氧化物或者金属氢化物分别与氮气进行原位反应,生成氮化物陶瓷;
步骤S5中,所述第二设定气氛为真空、氩气、氦气或氮气。
11.根据权利要求10所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,所述原料粉体的各粉体之间的摩尔比为1:1。
12.根据权利要求1-9任一项所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,步骤S1中,所述原料粉体还包括C粉或Si粉;
步骤S4中,所述第一设定气氛为真空、氩气、氦气或氮气;
在第一设定气氛下,各金属粉体、金属氧化物或者金属氢化物分别与C或Si进行原位反应,生成碳化物、氮化物、碳氮化物或硅化物陶瓷;
步骤S5中,所述第二设定气氛为真空、氩气、氦气或氮气。
13.根据权利要求12所述的高熵陶瓷惰性基弥散燃料芯块的制备方法,其特征在于,所述原料粉体中,各金属粉体之间的摩尔比为1:1,各金属氧化物粉体之间的摩尔比1:1,各金属氢化物粉体之间的摩尔比1:1;
所述C粉与各金属粉体或各金属氢化物粉体之间的摩尔比为1:1,所述C粉与各金属氧化物粉体之间的摩尔比为3:1;
所述Si粉与各金属粉体、各金属氧化物粉体或各金属氢化物粉体之间的摩尔比为1:1。
14.一种高熵陶瓷惰性基弥散燃料芯块,其特征在于,采用权利要求1-13任一项所述的制备方法制得。
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CN116199515A (zh) * 2023-02-23 2023-06-02 广东工业大学 一种碳化硅/高熵碳氮化物复合粉体及其制备方法和应用
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