CN112355311B - 一种钨基金属陶瓷核燃料芯块及其制备方法 - Google Patents
一种钨基金属陶瓷核燃料芯块及其制备方法 Download PDFInfo
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- CN112355311B CN112355311B CN202011128428.6A CN202011128428A CN112355311B CN 112355311 B CN112355311 B CN 112355311B CN 202011128428 A CN202011128428 A CN 202011128428A CN 112355311 B CN112355311 B CN 112355311B
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- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 title claims abstract description 174
- 229910052721 tungsten Inorganic materials 0.000 title claims abstract description 167
- 239000010937 tungsten Substances 0.000 title claims abstract description 167
- 229910052751 metal Inorganic materials 0.000 title claims abstract description 164
- 239000002184 metal Substances 0.000 title claims abstract description 164
- 239000000919 ceramic Substances 0.000 title claims abstract description 98
- 239000008188 pellet Substances 0.000 title claims abstract description 48
- 239000003758 nuclear fuel Substances 0.000 title claims abstract description 44
- 238000002360 preparation method Methods 0.000 title claims abstract description 12
- 239000011159 matrix material Substances 0.000 claims abstract description 38
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 62
- 239000000843 powder Substances 0.000 claims description 58
- OOAWCECZEHPMBX-UHFFFAOYSA-N oxygen(2-);uranium(4+) Chemical compound [O-2].[O-2].[U+4] OOAWCECZEHPMBX-UHFFFAOYSA-N 0.000 claims description 32
- FCTBKIHDJGHPPO-UHFFFAOYSA-N uranium dioxide Inorganic materials O=[U]=O FCTBKIHDJGHPPO-UHFFFAOYSA-N 0.000 claims description 32
- 239000011195 cermet Substances 0.000 claims description 29
- 229910045601 alloy Inorganic materials 0.000 claims description 28
- 239000000956 alloy Substances 0.000 claims description 28
- 239000012700 ceramic precursor Substances 0.000 claims description 24
- 229910052750 molybdenum Inorganic materials 0.000 claims description 20
- 239000011733 molybdenum Substances 0.000 claims description 20
- 239000002245 particle Substances 0.000 claims description 20
- 239000011241 protective layer Substances 0.000 claims description 19
- 238000005245 sintering Methods 0.000 claims description 16
- 238000002156 mixing Methods 0.000 claims description 15
- 238000000034 method Methods 0.000 claims description 13
- 239000000463 material Substances 0.000 claims description 10
- 239000011248 coating agent Substances 0.000 claims description 9
- 238000000576 coating method Methods 0.000 claims description 9
- 238000000465 moulding Methods 0.000 claims description 8
- 239000012298 atmosphere Substances 0.000 claims description 7
- 238000005260 corrosion Methods 0.000 claims description 6
- 230000007797 corrosion Effects 0.000 claims description 6
- 230000001681 protective effect Effects 0.000 claims description 4
- 229910052770 Uranium Inorganic materials 0.000 claims description 3
- 238000005229 chemical vapour deposition Methods 0.000 claims description 3
- 238000001755 magnetron sputter deposition Methods 0.000 claims description 3
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 claims description 3
- PONLSTWIGVAHBQ-UHFFFAOYSA-N azane plutonium Chemical compound N.[Pu] PONLSTWIGVAHBQ-UHFFFAOYSA-N 0.000 claims description 2
- MVXWAZXVYXTENN-UHFFFAOYSA-N azanylidyneuranium Chemical compound [U]#N MVXWAZXVYXTENN-UHFFFAOYSA-N 0.000 claims description 2
- 238000011049 filling Methods 0.000 claims description 2
- UTDLAEPMVCFGRJ-UHFFFAOYSA-N plutonium dihydrate Chemical compound O.O.[Pu] UTDLAEPMVCFGRJ-UHFFFAOYSA-N 0.000 claims description 2
- FLDALJIYKQCYHH-UHFFFAOYSA-N plutonium(IV) oxide Inorganic materials [O-2].[O-2].[Pu+4] FLDALJIYKQCYHH-UHFFFAOYSA-N 0.000 claims description 2
- 238000012545 processing Methods 0.000 claims description 2
- 238000007581 slurry coating method Methods 0.000 claims description 2
- 239000000446 fuel Substances 0.000 abstract description 7
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 10
- 229910026551 ZrC Inorganic materials 0.000 description 9
- OTCHGXYCWNXDOA-UHFFFAOYSA-N [C].[Zr] Chemical compound [C].[Zr] OTCHGXYCWNXDOA-UHFFFAOYSA-N 0.000 description 9
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 8
- 238000001035 drying Methods 0.000 description 8
- 239000007788 liquid Substances 0.000 description 8
- 229910017604 nitric acid Inorganic materials 0.000 description 8
- 238000002203 pretreatment Methods 0.000 description 8
- QAOWNCQODCNURD-UHFFFAOYSA-N sulfuric acid Substances OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 8
- 239000002243 precursor Substances 0.000 description 7
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 description 6
- 230000000052 comparative effect Effects 0.000 description 6
- 239000010410 layer Substances 0.000 description 6
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 5
- 238000004140 cleaning Methods 0.000 description 5
- 229910002804 graphite Inorganic materials 0.000 description 5
- 239000010439 graphite Substances 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
- 239000004005 microsphere Substances 0.000 description 5
- 238000007731 hot pressing Methods 0.000 description 4
- 239000002002 slurry Substances 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- 239000000758 substrate Substances 0.000 description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- 229910000691 Re alloy Inorganic materials 0.000 description 3
- 239000012300 argon atmosphere Substances 0.000 description 3
- 238000005520 cutting process Methods 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 239000011812 mixed powder Substances 0.000 description 3
- 238000005498 polishing Methods 0.000 description 3
- DECCZIUVGMLHKQ-UHFFFAOYSA-N rhenium tungsten Chemical compound [W].[Re] DECCZIUVGMLHKQ-UHFFFAOYSA-N 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- 238000005530 etching Methods 0.000 description 2
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 description 2
- 150000001247 metal acetylides Chemical class 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000003380 propellant Substances 0.000 description 2
- 238000001878 scanning electron micrograph Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000002344 surface layer Substances 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 1
- 241000282414 Homo sapiens Species 0.000 description 1
- 241000232219 Platanista Species 0.000 description 1
- 229910052778 Plutonium Inorganic materials 0.000 description 1
- 239000004372 Polyvinyl alcohol Substances 0.000 description 1
- 229910001080 W alloy Inorganic materials 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000013590 bulk material Substances 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000004992 fission Effects 0.000 description 1
- 238000001513 hot isostatic pressing Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- QGLKJKCYBOYXKC-UHFFFAOYSA-N nonaoxidotritungsten Chemical compound O=[W]1(=O)O[W](=O)(=O)O[W](=O)(=O)O1 QGLKJKCYBOYXKC-UHFFFAOYSA-N 0.000 description 1
- 238000013021 overheating Methods 0.000 description 1
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 description 1
- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
- 238000001272 pressureless sintering Methods 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 229910052702 rhenium Inorganic materials 0.000 description 1
- WUAPFZMCVAUBPE-UHFFFAOYSA-N rhenium atom Chemical compound [Re] WUAPFZMCVAUBPE-UHFFFAOYSA-N 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 238000002490 spark plasma sintering Methods 0.000 description 1
- MTPVUVINMAGMJL-UHFFFAOYSA-N trimethyl(1,1,2,2,2-pentafluoroethyl)silane Chemical compound C[Si](C)(C)C(F)(F)C(F)(F)F MTPVUVINMAGMJL-UHFFFAOYSA-N 0.000 description 1
- UONOETXJSWQNOL-UHFFFAOYSA-N tungsten carbide Chemical compound [W+]#[C-] UONOETXJSWQNOL-UHFFFAOYSA-N 0.000 description 1
- 229910001930 tungsten oxide Inorganic materials 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
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- B22F7/00—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression
- B22F7/06—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression of composite workpieces or articles from parts, e.g. to form tipped tools
- B22F7/08—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression of composite workpieces or articles from parts, e.g. to form tipped tools with one or more parts not made from powder
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Abstract
本发明公开了一种钨基金属陶瓷核燃料芯块及其制备方法，该芯块包括钨基金属陶瓷基体，所述钨基金属陶瓷基体上具有呈阵列式均匀排列的通孔结构，所述通孔结构的内壁具有保护层，且所述保护层将通孔结构的内壁完全覆盖。本发明避免了燃料芯块钨基金属陶瓷基体内部陶瓷相与外界环境的直接接触，起到保护作用，提高了钨基金属陶瓷核燃料芯块运行的安全可靠性。
Description
技术领域
本发明涉及核燃料技术领域，尤其涉及一种钨基金属陶瓷核燃料芯块及其制备方法。
背景技术
深空探测是人类最前沿的科技探索活动之一，不仅可加深人们对宇宙及生命的认识，还可推动空间科学、新材料等方面研究发展。传统的化学推进系统由于受到化学能限制，即便是最高效的液氢液氧发动机比冲仍无法达到500s，无法满足未来大载荷、载人深空探测任务的需求。因此，具有更高比冲的核推进系统成为未来深空探测主要甚至是唯一的选择。
自上世纪中期以来，美苏等国已在核热、核电推进空间发动机领域取得了一定的成果，先后研制并测试了多个系列的空间核动力发动机，而我国在该领域则起步较晚。2004年以来，随着嫦娥工程拉开了我国深空探测的序幕，火星探测、载人航天及空间站建设等任务也逐步展开，这对我国的空间核推进技术发展提出了迫切要求。
核热推进是利用核反应堆产生的裂变能将推进剂加热到高温高压状态，并将其从尾喷口喷出产生动力。因此在保证基体结构稳定的前提下，为有效实现热量传递，燃料芯块通常采用高熔点、高热导率及高硬度的钨基金属与燃料陶瓷进行混合，并设计成具备贯通孔的蜂窝状结构便于热量传导。然而，在极端高温高压工作条件下(达3000K)，包括热氢等在内的工质会与贯通孔中暴露在外界环境中的铀或钚基燃料陶瓷发生一定的副反应，导致燃料陶瓷结构破坏，甚至造成局部过热及燃料芯块结构破损，给安全性带来极大隐患。因此，如何实现钨基金属陶瓷燃料芯块安全可靠运行，成为亟待解决的一个重要难题。
发明内容
基于背景技术存在的技术问题，本发明提出了一种钨基金属陶瓷核燃料芯块及其制备方法。
本发明提出的一种钨基金属陶瓷核燃料芯块，包括钨基金属陶瓷基体，所述钨基金属陶瓷基体上具有呈阵列式均匀排列的通孔结构，所述通孔结构的内壁具有保护层，且所述保护层将通孔结构的内壁完全覆盖；
所述钨基金属陶瓷基体由陶瓷相与金属钨或者钨基合金组成，所述陶瓷相均匀弥散分布在基体中，其中陶瓷相包括二氧化铀、氮化铀、碳化铀、碳化钚、氮化钚、二氧化钚中的至少一种；
所述保护层由金属钨或者钨基合金组成。
优选地，所述保护层的厚度为0.1-1000μm。
优选地，所述钨基金属陶瓷基体中，陶瓷相的体积百分比为10-60％。
优选地，所述陶瓷相为颗粒状，粒径为10-500μm。
优选地，所述钨基合金为以金属钨为主要成分的合金；优选地，所述钨基合金中，钨的含量≥90wt％。
本发明中，钨基合金例如可以是钨与金属氧化物或者碳化物、铼、铝、铜中的至少一种组成的合金，其中金属氧化物或者碳化物的含量＜5wt％，所述金属氧化物或者碳化物包括氧化锆、氧化镧、氧化钇、氧化钨、碳化锆、碳化钛、碳化钨等中的至少一种。
一种所述的钨基金属陶瓷核燃料芯块的制备方法，包括下述步骤：
S1、将金属钼棒表面进行预处理，在其表面形成一层均匀的金属钨或者钨基合金涂层；
S2、将陶瓷相粉体与金属钨粉或者钨基合金粉按比例混合均匀，得到钨基金属陶瓷前驱粉体；
S3、用S1预处理后的金属钼棒和S2得到的钨基金属陶瓷前驱粉体填充模具，使预处理后的金属钼棒呈阵列式均匀排列在钨基金属陶瓷前驱粉体中，经过冷压成型，得到坯体；
S4、将所述坯体在真空或保护气氛下烧结，得到块材；
S5、将所述块材进行机械加工，使得金属钼棒两端暴露，通过腐蚀完全去除块材中的金属钼棒，得到钨基金属陶瓷核燃料芯块。
优选地，所述步骤S3中，先在模具底部平铺一层钨基金属陶瓷前驱粉体，然后在粉体上均匀放置预处理后的金属钼棒，按照一层钨基金属陶瓷前驱粉体一层预处理后的金属钼棒的方式填充模具，最后在最上层平铺一层钨基金属陶瓷前驱粉体，经过冷压成型，得到坯体。
优选地，所述步骤S1中，金属钼棒表面进行预处理的方法为磁控溅射、化学气相沉积、浆料涂覆中的至少一种。
优选地，所述步骤S4中，烧结温度为1600-2200℃，烧结时间为0.1-20h；优选地，所述烧结方法为无压烧结、热压烧结、热等静压烧结或者放电等离子体烧结，所述保护气氛为氢气气氛、氩气气氛、氮气气氛中的至少一种。
优选地，所述步骤S5中，腐蚀去除块材中金属钼的具体方法如下：将块材进行切割，使得金属钼棒两端暴露，然后置于腐蚀液中，通过腐蚀完全去除金属钼棒。
优选地，所述腐蚀液的组分包括浓硝酸与浓硫酸、氢氟酸、浓盐酸中至少一种的组合；优选地，所述腐蚀液的组分包括浓硝酸、浓硫酸、氢氟酸、浓盐酸，其中浓硝酸、浓硫酸、氢氟酸、浓盐酸的体积比为(3-8)：(1-5)：(0-3)：(0-5)。
本发明的有益效果如下：
本发明通过对金属钼棒表层进行预处理，并结合选择性腐蚀工艺，实现在钨基金属陶瓷贯通孔内壁形成一定厚度的保护层。其方法是在制备具有通孔的钨基金属陶瓷过程中，通过在金属钼棒表层涂覆或溅射一层金属钨和/或钨基合金涂层，并将其置于金属钨粉或者钨基合金粉与陶瓷相组成的钨基金属陶瓷前驱混合粉体中，烧结后利用腐蚀液选择性腐蚀去除金属钼棒部分，从而在形成通孔的同时，在通孔内壁也形成具有一定厚度的保护层，避免了燃料芯块钨基金属陶瓷基体内部陶瓷相与外界环境的直接接触，起到保护作用，提高了钨基金属陶瓷核燃料芯块运行的安全可靠性。本发明的方法操作简单且易实现工业化，具有广阔的应用前景。
附图说明
图1为本发明实施例1中钨基金属陶瓷核燃料芯块的制备流程示意图。
图2为本发明实施例1中金属钼棒预处理前后的对比图，左边为金属钼棒预处理前的图片，右边为金属钼棒预处理后的图片。
图3为本发明实施例1中钨基金属陶瓷核燃料芯块扫描电镜照片。
图4为本发明实施例2中钨基金属陶瓷核燃料芯块的扫描电镜照片。
图5为本发明对比例1中钨基金属陶瓷核燃料芯块的断面显微照片。
图6为本发明对比例2中钨基金属陶瓷核燃料芯块的断面显微照片。
具体实施方式
下面，通过具体实施例对本发明的技术方案进行详细说明。
实施例1
一种钨基金属陶瓷核燃料芯块，包括钨基金属陶瓷基体，钨基金属陶瓷基体上具有呈阵列式均匀排列的通孔结构，通孔结构的内壁具有保护层，且保护层将通孔结构的内壁完全覆盖；
钨基金属陶瓷基体由二氧化铀陶瓷相与金属钨组成，其中二氧化铀陶瓷相呈颗粒状均匀弥散分布在基体中，其粒径为180μm；钨基金属陶瓷基体中，二氧化铀陶瓷相的体积百分比为55％；
保护层由金属钨组成，厚度为10μm。
钨基金属陶瓷核燃料芯块的制备方法，包括下述步骤：
S1、通过浆料涂覆-烘干方法对直径为2mm、长度为2cm的金属钼棒表面进行预处理，在其表面形成一层均匀的金属钨涂层；
S2、将粒径为180μm的二氧化铀微球与粒径为550nm的金属钨粉按体积比为5.5：4.5混合均匀，得到钨基金属陶瓷前驱粉体；
S3、将15g S2得到的钨基金属陶瓷前驱粉体平铺在内径为Φ30mm，外径为Φ50mm，高度为10cm的圆柱形石墨模具底部，然后在粉体上均匀放置5根S1预处理后的金属钼棒，再平铺20g S2得到的钨基金属陶瓷前驱粉体，然后在其上均匀放置5根S1预处理后的金属钼棒，再在其上平铺20g S2得到的钨基金属陶瓷前驱粉体，然后在其上均匀放置5根S1预处理后的金属钼棒，最后在其上平铺20g S2得到的钨基金属陶瓷前驱粉体，经过冷压成型，得到坯体；
S4、将模具置于放电等离子体烧结炉中，在氩气气氛下于1750℃、40MPa下烧结15min，得到块材；
S5、将块材进行切割，使得金属钼棒两端暴露，然后置于浓度为68％的浓硝酸和浓度为98％的浓硫酸按体积比1：1混合得到的腐蚀液中，加热至70℃腐蚀完全去除块材中的金属钼棒，清洗、干燥后得到钨基金属陶瓷核燃料芯块。
S1中，浆料涂覆-烘干的方法具体为：将金属钨粉与聚乙烯醇水溶液混合得到浆料，再将浆料均匀涂覆在金属钼棒表面，烘干，即可。
实施例2
一种钨基金属陶瓷核燃料芯块，包括钨基金属陶瓷基体，钨基金属陶瓷基体上具有呈阵列式均匀排列的通孔结构，通孔结构的内壁具有保护层，且保护层将通孔结构的内壁完全覆盖；
钨基金属陶瓷基体由二氧化铀陶瓷相与钨基合金组成，其中二氧化铀陶瓷相呈颗粒状均匀弥散分布在基体中，其粒径为200μm；钨基金属陶瓷基体中，二氧化铀陶瓷相的体积百分比为50％；钨基合金由钨与碳化锆组成，碳化锆占钨基合金总质量的0.5wt％；
保护层由钨铼合金W90Re10组成，厚度为1μm。
钨基金属陶瓷核燃料芯块的制备方法，包括下述步骤：
S1、通过磁控溅射方法对直径为2mm、长度为5cm的金属钼棒表面进行预处理，在其表面形成一层均匀的钨铼合金W90Re10涂层；
S2、将粒径为200μm的二氧化铀微球与粒径为500nm的钨基合金粉按体积比为5：5混合均匀，得到钨基金属陶瓷前驱粉体，其中钨基合金粉的成分由钨与碳化锆组成，碳化锆占钨基合金粉总质量的0.5wt％；
S3、将130g S2得到的钨基金属陶瓷前驱粉体平铺在内径为Φ60mm，外径为Φ120mm，高度为10cm的圆柱形石墨模具底部，然后在粉体上均匀放置3根S1预处理后的金属钼棒，再在其上平铺130g S2得到的钨基金属陶瓷前驱粉体，经过冷压成型，得到坯体；
S4、将模具置于热压炉中，在真空气氛下于1800℃、32MPa下烧结1h，得到块材；
S5、将块材进行打磨，使得金属钼棒两端暴露，然后置于浓度为68％的浓硝酸、浓度为98％的浓硫酸、浓度为37％的浓盐酸、水按5:3:1:1体积比混合得到的腐蚀液中，加热至70℃腐蚀完全去除块材中的金属钼棒，清洗、干燥后得到钨基金属陶瓷核燃料芯块。
实施例3
一种钨基金属陶瓷核燃料芯块，包括钨基金属陶瓷基体，钨基金属陶瓷基体上具有呈阵列式均匀排列的通孔结构，通孔结构的内壁具有保护层，且保护层将通孔结构的内壁完全覆盖；
钨基金属陶瓷基体由二氧化铀陶瓷相与金属钨组成，其中二氧化铀陶瓷相呈颗粒状均匀弥散分布在基体中，其粒径为180μm；钨基金属陶瓷基体中，二氧化铀陶瓷相的体积百分比为50％；
保护层由金属钨组成，厚度为0.5μm。
钨基金属陶瓷核燃料芯块的制备方法，包括下述步骤：
S1、通过化学气相沉积方法对直径为2mm、长度为5cm的金属钼棒表面进行预处理，在其表面形成一层均匀的金属钨涂层；
S2、将粒径为180μm的二氧化铀微球与粒径为2.8μm的金属钨粉按体积比为5：5混合均匀，得到钨基金属陶瓷前驱粉体；
S3、将180g S2得到的钨基金属陶瓷前驱粉体平铺在内径为Φ60mm，外径为Φ120mm，高度为16cm的圆柱形石墨模具底部，然后在粉体上均匀放置3根S1预处理后的金属钼棒，再平铺180g S2得到的钨基金属陶瓷前驱粉体，然后在其上均匀放置4根S1预处理后的金属钼棒，再平铺180g S2得到的钨基金属陶瓷前驱粉体，然后在其上均匀放置3根S1预处理后的金属钼棒，最后平铺180g S2钨基金属陶瓷前驱粉体，经过冷压成型，得到坯体；
S4、将模具置于热压炉中，在真空气氛下于1800℃、30MPa下烧结1h，得到块材；
S5、将块材进行打磨，使得金属钼棒两端暴露，然后置于浓度为68％的浓硝酸、浓度为98％的浓硫酸、水按体积比5:3:2混合得到的腐蚀液中，加热至60℃腐蚀完全去除块材中的金属钼棒，清洗、干燥后得到钨基金属陶瓷核燃料芯块。
对比例1
一种钨基金属陶瓷核燃料芯块，包括钨基金属陶瓷基体，钨基金属陶瓷基体上具有呈阵列式均匀排列的通孔结构；
钨基金属陶瓷基体由二氧化铀陶瓷相与金属钨组成，其中二氧化铀陶瓷相呈颗粒状均匀弥散分布在基体中，粒径为180μm；钨基金属陶瓷基体中，二氧化铀陶瓷相的体积百分比为55％；
钨基金属陶瓷核燃料芯块的制备方法，包括下述步骤：
(1)将粒径为180μm的二氧化铀微球与粒径为550nm的金属钨粉按体积比为5.5：4.5混合均匀，得到钨基金属陶瓷前驱粉体；
(2)将15g S1得到的钨基金属陶瓷前驱粉体平铺在内径为Φ30mm，外径为Φ50mm，高度为10cm的圆柱形石墨模具底部，然后在粉体上均匀放置5根金属钼棒，再平铺20g S1得到的钨基金属陶瓷前驱粉体，然后在其上均匀放置5根金属钼棒，再在其上平铺20g S1得到的钨基金属陶瓷前驱粉体，然后在其上均匀放置5根金属钼棒，最后在其上平铺20g S1得到的钨基金属陶瓷前驱粉体，经过冷压成型，得到坯体，其中金属钼棒的直径为2mm、长度为2cm；
(3)将模具置于放电等离子体烧结炉中，在氩气气氛下于1750℃、40MPa下烧结15min，得到块材；
(4)将块材进行切割，使得金属钼棒两端暴露，然后置于浓度为68％的浓硝酸和浓度为98％的浓硫酸按体积比1：1混合得到的腐蚀液中，加热至70℃腐蚀完全去除块材中的金属钼棒，清洗、干燥后得到钨基金属陶瓷核燃料芯块。
对比例2
一种钨基金属陶瓷核燃料芯块，包括钨基金属陶瓷基体，钨基金属陶瓷基体上具有呈阵列式均匀排列的通孔结构；
钨基金属陶瓷基体由二氧化铀陶瓷相与钨基合金组成，其中二氧化铀陶瓷相均匀弥散分布在基体中，其粒径为200μm；钨基金属陶瓷基体中，二氧化铀陶瓷相的体积百分比为50％；钨基合金由钨与碳化锆组成，碳化锆占钨基合金总质量的0.5wt％；
钨基金属陶瓷核燃料芯块的制备方法，包括下述步骤：
(1)将粒径为200μm的二氧化铀微球与粒径为500nm的钨基合金粉按体积比为5：5混合均匀，得到钨基金属陶瓷前驱粉体，其中钨基合金粉的成分由钨与碳化锆组成，碳化锆占钨基合金粉总质量的0.5wt％；
(2)将130g S1得到的钨基金属陶瓷前驱粉体平铺在内径为Φ60mm，外径为Φ120mm，高度为10cm的圆柱形石墨模具底部，然后在粉体上均匀放置3根直径为2mm、长度为5cm的金属钼棒，再在其上平铺130g S1得到的钨基金属陶瓷前驱粉体，经过冷压成型，得到坯体；
(3)将坯体置于热压炉中，在真空气氛下于1800℃、32MPa下烧结1h，得到块材；
(4)将块材进行打磨，使得金属钼棒两端暴露，然后置于浓度为68％的浓硝酸、浓度为98％的浓硫酸、浓度为37％的浓盐酸、水按5:3:1:1体积比混合得到的腐蚀液中，加热至70℃腐蚀完全去除块材中的金属钼棒，清洗、干燥后得到钨基金属陶瓷核燃料芯块。
图2为本发明实施例1中金属钼棒预处理前后的对比图，左边为金属钼棒预处理前的图片，右边为金属钼棒预处理后的图片。参照图2，预处理前金属钼棒表面呈银白色，经过预处理后得到表面具有金属钨涂层的金属钼棒，呈黑色。将其放置于钨基金属陶瓷混合粉体中高温烧结后形成致密块材，进一步通过腐蚀液腐蚀后，钼基金属溶解于腐蚀液中，而钨基金属陶瓷部分保持结构完好，最终可以形成通孔内壁具备金属钨保护层的蜂窝状钨基金属陶瓷块材。
图3为本发明实施例1中钨基金属陶瓷核燃料芯块扫描电镜照片。由图3可见，椭球形二氧化铀颗粒均匀分布于钨基金属陶瓷基体中，钨基金属陶瓷基体中具有通孔，且由于通孔内壁被金属钨保护层包围，未出现二氧化铀颗粒与通孔内壁直接接触的现象。
图4为本发明实施例2中钨基金属陶瓷核燃料芯块的扫描电镜照片。由图4可见，椭球形二氧化铀颗粒均匀分布于钨基金属陶瓷基体中，钨基金属陶瓷基体中具有通孔，且由于通孔内壁被钨铼合金保护层包围，未出现二氧化铀颗粒与通孔内壁直接接触的现象。
图5为本发明对比例1中钨基金属陶瓷核燃料芯块的断面显微照片。由图5可见，部分椭球形二氧化铀颗粒直接暴露于通孔内壁中。
图6为本发明对比例2中钨基金属陶瓷核燃料芯块的断面显微照片。由图6可见，部分椭球形二氧化铀颗粒直接暴露于通孔内壁中。
以上所述，仅为本发明较佳的具体实施方式，但本发明的保护范围并不局限于此，任何熟悉本技术领域的技术人员在本发明揭露的技术范围内，根据本发明的技术方案及其发明构思加以等同替换或改变，都应涵盖在本发明的保护范围之内。
Claims (8)
1.一种钨基金属陶瓷核燃料芯块，其特征在于，包括钨基金属陶瓷基体，所述钨基金属陶瓷基体上具有呈阵列式均匀排列的通孔结构，所述通孔结构的内壁具有保护层，且所述保护层将通孔结构的内壁完全覆盖；
所述钨基金属陶瓷基体由陶瓷相与金属钨或者钨基合金组成，所述陶瓷相均匀弥散分布在基体中，其中陶瓷相包括二氧化铀、氮化铀、碳化铀、碳化钚、氮化钚、二氧化钚中的至少一种；
所述保护层由金属钨或者钨基合金组成。
2.根据权利要求1所述的钨基金属陶瓷核燃料芯块，其特征在于，所述保护层的厚度为0.1-1000μm。
3.根据权利要求1或2所述的钨基金属陶瓷核燃料芯块，其特征在于，所述钨基金属陶瓷基体中，陶瓷相的体积百分比为10-60％。
4.根据权利要求1或2所述的钨基金属陶瓷核燃料芯块，其特征在于，所述陶瓷相为颗粒状，粒径为10-500μm。
5.根据权利要求1或2所述的钨基金属陶瓷核燃料芯块，其特征在于，所述钨基合金为以金属钨为主要成分的合金，其中钨的含量≥90wt％。
6.一种如权利要求1-5任一项所述的钨基金属陶瓷核燃料芯块的制备方法，其特征在于，包括下述步骤：
S1、将金属钼棒表面进行预处理，在其表面形成一层均匀的金属钨或者钨基合金涂层；
S2、将陶瓷相粉体与金属钨粉或者钨基合金粉按比例混合均匀，得到钨基金属陶瓷前驱粉体；
S3、用S1预处理后的金属钼棒和S2得到的钨基金属陶瓷前驱粉体填充模具，使预处理后的金属钼棒呈阵列式均匀排列在钨基金属陶瓷前驱粉体中，经过冷压成型，得到坯体；
S4、将所述坯体在真空或保护气氛下烧结，得到块材；
S5、将所述块材进行机械加工，使得金属钼棒两端暴露，通过腐蚀完全去除块材中的金属钼棒，得到钨基金属陶瓷核燃料芯块。
7.根据权利要求6所述的钨基金属陶瓷核燃料芯块的制备方法，其特征在于，所述步骤S1中，金属钼棒表面进行预处理的方法为磁控溅射、化学气相沉积、浆料涂覆中的至少一种。
8.根据权利要求6或7所述的钨基金属陶瓷核燃料芯块的制备方法，其特征在于，所述步骤S4中，烧结温度为1600-2200℃，烧结时间为0.1-20h。
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