CN102246244A - 废料储存容器及其组合物 - Google Patents
废料储存容器及其组合物 Download PDFInfo
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- G21F1/00—Shielding characterised by the composition of the materials
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- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B28/00—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements
- C04B28/34—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements containing cold phosphate binders
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- C04B2111/00—Mortars, concrete or artificial stone or mixtures to prepare them, characterised by specific function, property or use
- C04B2111/00241—Physical properties of the materials not provided for elsewhere in C04B2111/00
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- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
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Abstract
提供了废料储存容器,由包含硅酸钙、氧化镁或氧化钙和酸式磷酸盐的组合物形成。该组合物也可以包含粉煤灰或高岭土,含有或不含硅酸钙。
Description
相关申请
本申请要求对2008年10月6日提交的美国临时专利申请No.61/102,997的优先权,该申请的内容以参考文献的方式完整地并入本文中。
发明的技术领域和背景技术
本发明主要涉及废料储存容器及其中有用的组合物,并尤其针对危险和/或放射性废料的储存。
混凝土或水泥通常是储存放射性废料的可选材料。例如,美国专利No.5,786,611号提出的储存核废料的容器。该容器包括具有稳定的氧化铀集料和中子吸收材料如B2O3、HfO3或Gd2O3的混凝土。美国专利No.4,257,912、4,326,918、4,845,372和4,950,246提出储存核废料的混凝土封装。美国专利No.5,402,455提出以多层的基于混凝土的储存容器来储存危险的、具有放射性的和混合的废料。
然而依然需要用作废料储存容器的组合物更便宜,更少依赖于复杂的密封系统,同时能屏蔽废料对环境的危害在可以接受的水平。
发明内容
本发明提供的废料储存容器组合物包含硅酸钙、氧化镁和酸式磷酸盐(acid phosphate)。
在另一个实施方案中,本发明提供的废料储存容器组合物包含氧化镁或氧化钙、酸式磷酸盐和粉煤灰。
在又一个实施方案中,本发明提供的废料储存容器组合物包含氧化镁或氧化钙、酸式磷酸盐和高岭土。基于0.662MeV(5μCi Cs-137源)和1.173MeV(1μCi Co-60源)的光子能量,这些容器与普通混凝土相比都具有改善的衰减系数。
附图说明
图1是在使用5mCi Cs-137源的0.666MeV的光子能量下,适合用于废料容器并示例在实施例1至实施例6中的的组合物与普通混凝土(“OC”)的衰减系数图。
图2是在使用1μCiCo-60源的1.173MeV的光子能量下,适合用于废料容器并示例在实施例1至实施例6中的的组合物与普通混凝土(“OC”)的衰减系数图。
具体实施方式
关于此处描述的其它实施方案,本发明前述及其他方面将进行详细的描述。请注意本发明可以使用不同的形式实施,而不仅限于在此陈述的实施方案。也就是说,提供这些实施方案是为了向本领域技术人员彻底地、完全地揭示本发明的范围。
对本发明进行描述时所使用的术语仅仅是为了描述特定的实施方案,不应当认为是对本发明的限制。在本发明的实施方案以及附加的权利要求中,除非上下文清楚表明的,单数形式的“一”(a,an)、“该”(the)包括复数形式。同样,文件中使用的“和/或”指的是并包含一个或多个相关项目的所有可能组合。此外,此文件中使用的术语“约”应用于可测量的值时,如组合物的数量、剂量、时间、温度等时,是包含该特定值的20%、10%、5%、1%、0.5%或甚至0.1%的偏差。除非有另外的规定,在说明书中使用的包括技术术语和科学术语的所有术语具有本发明所属领域内的普通技术人员所通常理解的含义。引用的所有文献都以全文引入以供参考。
废料容器可包含硅酸钙(硅灰石)、氧化镁和酸式磷酸盐。在一个实施方案中,该容器的组合物包含约15到40重量%的硅酸钙、约10到35重量%的氧化镁和约25到45重量%的酸式磷酸盐。该组合物中可任选地包含0.1%到40重量%的高岭土和/或粉煤灰。
在另一个实施方案中,废料容器包含氧化镁或氧化钙、酸式磷酸盐和粉煤灰。在一个实施方案中,该容器的组合物包含15到40重量%的煅烧氧化镁或氧化钙、25到55重量%的酸式磷酸盐和20到40重量%的粉煤灰。任选的含有0.1到40重量%的高岭土。
在又一个实施方案中,废料容器包含氧化镁或氧化钙、酸式磷酸盐和高岭土。在一个实施方案中,该容器的组合物包含15到40重量%的煅烧氧化镁或氧化钙、20到55重量%的酸式磷酸盐和5到25重量%的高岭土。可以任选的含有0.1%到40%重量的粉煤灰。
本发明包括的储存废料的方法包括由一种或多种上述的组合物来封装废料。
典型的酸式磷酸盐包括磷酸二氢钾、磷酸镁、磷酸钠、磷酸铝、磷酸铵、磷酸铁、磷酸锌及其组合。在上述的实施方案中,酸式磷酸盐可以是磷酸二氢钾。
典型的待储存废料包括危险废料、放射性废料和含危险废料和放射性废料的混合废料。这些废料的典型来源为废核燃料和核燃料电池。由上述组合物形成的废料储存容器可以根据需要的储存构造设计成多种几何形状(如圆形、方形、圆柱形、六边形等)。储存容器可以由上述的一种或多种组合物单独制成以封装待储存废料。另一种选择是,该容器可以包括由或没有屏蔽特性的任意材料制成的外壳和封装废料的一种或多种上述组合物。在另一个实施方案中,该容器可以包括外部非屏蔽材料、由非屏蔽材料形成的内壳和封装内壳的一种或多种上述组合物。此外,废料容器可以兼有辐射屏蔽性,如2009年10月2日提交的美国系列No.__相关申请(代理人卷号No.9591-7)中所描述的。该申请的公开部分以全文引用的形式并入本文以供参考。
辐射屏蔽结构组合物可以混合适当的添加剂,通常情况下添加剂的重量为约0.1到约30重量%。典型的添加剂包括阻燃剂、蛭石、珍珠岩、纤维、乳化剂、抗凝剂、螯合剂、粒状添加剂、石块或沙粒等粗集料、硼酸等化学添加剂、促进剂(如The Euclid Chemical Company,Cleveland,Ohio生产的Accelguard)、着色剂和颜料、填料、集料、硼砂、硅土料、铁氧化物、胶粘剂(如The Euclid Chemical Company,Cleveland,Ohio生产的Eucopoxy树脂和Eucoweld、Flexcon和Corr-bond)、塑化剂、硬化剂(如The Euclid ChemicalCompany,Cleveland,Ohio生产的Euco Diamond Hard)、修补聚合物(如The EuclidChemical Company,Cleveland,Ohio生产的Eucorapid补料(Eucorapid patch))、微二氧化硅粉(如The Euclid Chemical Company,Cleveland,Ohio生产的Eucoshot)、缓凝剂、表面软化剂、和高岭土、固化化合物(如Brownstone CS)、减水剂(如Accelguard,Eucon AC)及空气夹带剂(如AEA和Air Mix)。
或者,在辐射屏蔽结构组合物中也可添加中子吸收剂。典型的中子吸收剂包括重金属和重金属化合物例如硼、B2O3、HfO3、Gd2O3、氧化铁、铅等。
或者,在该组合物中可以添加各种加固成分(reinforcement),或者该组合物可用于加固成分。典型的加固成分包括钢(例如钢筋)、其他金属(例如铅)、碳、聚合物、玻璃、石料、玄武岩等,其为纤维、颗粒和/或织物/垫的形式。
以下实施例仅用于阐释本发明,并不限于此。
实施例
实施例1-6组成如下:
实施例1
氧化镁 23%
磷酸二氢钾 23%
粉煤灰 21%
沙 33%
实验样品厚度为0.50英寸。
实施例2
氧化镁 20%
磷酸二氢钾 23%
硅酸钙 24%
沙 33%
实验样品厚度为1.25英寸。
实施例3
重复实施例1,除了加入盐水。实验样品厚度为2.00英寸。
实施例4
实验样品厚度为0.75英寸。
实施例5
氧化镁 30%
磷酸二氢钾 34%
硅酸钙 36%
实验样品厚度为0.50英寸。
实施例6
氧化镁 30%
磷酸二氢钾 31%
粉煤灰 28%
碳酸氢钠 10%
实验样品厚度为1.00英寸。
实施例7
重复实施例1,实验样品厚度为1.00英寸。实验使用由North Carolina StateUniversity开发的测量衰减系数的方法。
由图1和图2可以看出,实施例1-6的配方设计与普通的混凝土相比,衰减系数有了明显改善。
实施例8
配方如下:
氧化镁 34%
磷酸二氢钾 31%
粉煤灰 17%
高岭土 15%
实施例9
将都嵌入了钢筋的实施例8与预拌混凝土(Ready Mix cement)进行加速腐蚀测试并比较。将样品浸入带电酸性浴,大约100小时后,预拌混凝土显示有显著裂缝,而500小时后,实施例8的组合物仍无裂缝呈现。
使用ASTMD5084对实施例8进行水力传导试验显示约4到5英寸的屏障足够保障300+年。
对实施例8、实施例9和预拌混凝土样本进行了氯化物离子试验和耐压强度试验(ASTM C109),结果如表1所示。
平均总重量 | 平均吸收的氯化物 | 耐压强度 | |
实施例8 | 0.91% | 0.13% | 8410(3天) |
实施例9 | 1.24% | 0.22% | 8000(3天) |
预拌混凝土 | 1.38% | 0.36% | 4440(28天) |
中子衰减
在实施例5中加入作为集料的富含硼的石材,制成两个圆柱,一个8英寸,另一个16英寸。中子衰减活性用PuBe中子源来测量,该中子源在1到10MeV范围内产生中子,平均能量为4.2MeV。用博纳球(Boner Sphere)中子谱仪在中子源与探测器的距离为30”时探测中子。这些圆柱体作为一个8”圆柱,以及两个合起来(即16”圆柱)被检测(投放了剂量),并与空白(无剂量)检测到的比较。在这项试验中所得剂量是空白处为9.2mRem/小时,8”圆柱为3.0mRem/小时,16”圆柱为2.6mRem/小时。屏蔽值证明了8”圆柱有67%的衰减而16”圆柱有72%的衰减。
中子的衰减通常以十分之一值层(tenth-value layers,TVL)为单位进行描述。这些数据预测出4.2MeV下的8”圆柱的TVL是40厘米。比较之下,用来屏蔽能量范围在0.5MeV内的医疗线性加速器产生的光中子的普通混凝土的典型十分之一值层为22厘米。中子衰减改善了。
上描述了本发明的某些实施方案,需要理解的是,由随后的权利要求所定义的本发明不受前文上述描述中的具体细节所限制,因为在不脱离随后的权利要求的实质或范围的前提下,可能会有多种明显的变体。
Claims (9)
1.废料储存容器,含有硅酸钙、氧化镁和酸式磷酸盐。
2.权利要求1的废料储存容器,含有10到40重量%的硅酸钙、10到35重量%的氧化镁和15到45重量%的酸式磷酸盐。
3.权利要求2的废料储存容器,其中的酸式磷酸盐是磷酸二氢钾。
4.废料储存容器,含有氧化镁或氧化钙、酸式磷酸盐和粉煤灰。
5.权利要求4的废料储存容器,含有15到35重量%的煅烧氧化镁或氧化钙、15到55重量%的酸式磷酸盐和20到40重量%的粉煤灰。
6.权利要求5的废料储存容器,其中酸式磷酸盐是磷酸二氢钾。
7.废料储存容器,含有氧化镁或氧化钙、酸式磷酸盐和高岭土。
8.权利要求7的废料储存容器,含有15到35重量%的煅烧氧化镁或氧化钙、15到55重量%的酸式磷酸盐和20到40重量%的高岭土。
9.权利要求8的废料储存容器,其中的酸式磷酸盐是磷酸二氢钾。
Applications Claiming Priority (5)
Application Number | Priority Date | Filing Date | Title |
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US10299708P | 2008-10-06 | 2008-10-06 | |
US61/102997 | 2008-10-06 | ||
US12/572,812 US8409346B2 (en) | 2008-10-06 | 2009-10-02 | Waste storage vessels and compositions therefor |
US12/572812 | 2009-10-02 | ||
PCT/US2009/059477 WO2010042417A2 (en) | 2008-10-06 | 2009-10-05 | Waste storage vessels and compositions therefor |
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CN2009801488255A Pending CN102246244A (zh) | 2008-10-06 | 2009-10-05 | 废料储存容器及其组合物 |
CN2009801488274A Pending CN102246245A (zh) | 2008-10-06 | 2009-10-05 | 辐射屏蔽结构组合物 |
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KR (2) | KR20110084417A (zh) |
CN (2) | CN102246244A (zh) |
BR (2) | BRPI0920813A2 (zh) |
CA (2) | CA2742305A1 (zh) |
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US20100090168A1 (en) * | 2008-10-06 | 2010-04-15 | Grancrete, Inc. | Radiation shielding structure composition |
CN102276207B (zh) * | 2011-06-28 | 2013-05-08 | 中国核工业华兴建设有限公司 | 一种硅铁牺牲混凝土 |
JP2013061287A (ja) * | 2011-09-14 | 2013-04-04 | Kawahara Technical Research Inc | ペースト製造方法およびペースト |
JP5285173B2 (ja) * | 2011-09-14 | 2013-09-11 | 株式会社カワハラ技研 | 放射線防護服および宇宙服 |
JP5248702B2 (ja) * | 2011-09-14 | 2013-07-31 | 株式会社カワハラ技研 | 生命維持装置 |
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US20150041723A1 (en) * | 2012-02-27 | 2015-02-12 | The Regents Of The University Of California | Chemically bonded ceramics based on boron and lead |
KR101319256B1 (ko) | 2012-03-05 | 2013-10-17 | 주식회사 경동나비엔 | 연소기기용 가스 공기 혼합장치 |
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- 2009-10-02 US US12/572,812 patent/US8409346B2/en not_active Expired - Fee Related
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- 2009-10-05 BR BRPI0920813A patent/BRPI0920813A2/pt not_active IP Right Cessation
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- 2009-10-05 CN CN2009801488274A patent/CN102246245A/zh active Pending
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EP2345042A4 (en) | 2012-06-27 |
US8409346B2 (en) | 2013-04-02 |
BRPI0920603A2 (pt) | 2015-12-22 |
KR20110084416A (ko) | 2011-07-22 |
JP2012504773A (ja) | 2012-02-23 |
TW201019347A (en) | 2010-05-16 |
TW201019348A (en) | 2010-05-16 |
WO2010042417A3 (en) | 2010-07-08 |
EP2345042A2 (en) | 2011-07-20 |
CN102246245A (zh) | 2011-11-16 |
JP2012504774A (ja) | 2012-02-23 |
WO2010042416A2 (en) | 2010-04-15 |
KR20110084417A (ko) | 2011-07-22 |
EP2345043A2 (en) | 2011-07-20 |
WO2010042417A2 (en) | 2010-04-15 |
EP2345043A4 (en) | 2012-06-20 |
US20140061542A1 (en) | 2014-03-06 |
CA2742305A1 (en) | 2010-04-15 |
US20100090168A1 (en) | 2010-04-15 |
CA2742259A1 (en) | 2010-04-15 |
WO2010042416A3 (en) | 2010-07-08 |
US20100089292A1 (en) | 2010-04-15 |
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