CN106133844B - 熔盐反应堆中的化学优化 - Google Patents
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Classifications
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- G21C—NUCLEAR REACTORS
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- G21C17/02—Devices or arrangements for monitoring coolant or moderator
- G21C17/022—Devices or arrangements for monitoring coolant or moderator for monitoring liquid coolants or moderators
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- G21C3/02—Fuel elements
- G21C3/04—Constructional details
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- G—PHYSICS
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- G21C—NUCLEAR REACTORS
- G21C1/00—Reactor types
- G21C1/02—Fast fission reactors, i.e. reactors not using a moderator ; Metal cooled reactors; Fast breeders
- G21C1/03—Fast fission reactors, i.e. reactors not using a moderator ; Metal cooled reactors; Fast breeders cooled by a coolant not essentially pressurised, e.g. pool-type reactors
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
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- G21C15/00—Cooling arrangements within the pressure vessel containing the core; Selection of specific coolants
- G21C15/28—Selection of specific coolants ; Additions to the reactor coolants, e.g. against moderator corrosion
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- G21C3/041—Means for removal of gases from fuel elements
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- G—PHYSICS
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- G21C—NUCLEAR REACTORS
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- G21C3/02—Fuel elements
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- G—PHYSICS
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- G21C—NUCLEAR REACTORS
- G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
- G21C3/02—Fuel elements
- G21C3/04—Constructional details
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- G—PHYSICS
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- G21C—NUCLEAR REACTORS
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- G21C3/02—Fuel elements
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- G21C3/16—Details of the construction within the casing
- G21C3/17—Means for storage or immobilisation of gases in fuel elements
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
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Abstract
牺牲金属在含有锕系元素卤化物的熔盐燃料的核裂变反应堆中的用途,所述用途为了在没有将锕系元素三卤化物还原为锕系金属的情况下维持锕系元素三卤化物与锕系元素四卤化物的预定比率。一种维持含有锕系元素卤化物的熔盐的氧化态的方法。所述方法包括使所述熔盐连续地与牺牲金属接触,对所述牺牲金属进行选择以便在没有将锕系元素三卤化物还原为锕系金属的情况下维持锕系元素三卤化物与锕系元素四卤化物的预定比率。还描述了一种含有牺牲金属的燃料管。
Description
技术领域
本发明涉及用于裂变反应堆(fission reactor)的熔盐燃料(molten salt fuel)的化学优化(chemical optimisation)。
背景
使用熔融卤化物盐形式的裂变燃料的核裂变反应堆与固体燃料反应堆相比具有许多优点,但是通常遇到由于随着裂变产物累积和卤素从锕系元素三或四卤化物燃料中的净释放发生,在运行期间熔融燃料盐的化学组成的连续变化所致的问题。熔盐反应堆的大多数设计在燃料循环中结合连续化学处理过程以应付该问题,然而这么做涉及将复杂的化学工程系统添加到高度放射性环境中。
在GB 2508537中描述了简单得多的熔盐反应堆的设计,其中将燃料盐容纳在静止管中,在该静止管中对流或其他混合过程允许热量以对于反应堆来说足够的速率从燃料盐传给管壁以具有实际能量产生。这样的静止燃料管不允许燃料盐的化学性质的连续主动调节。在GB 2508537中,提议了在燃料盐中或在燃料管上包含金属如铌、钛或镍将会在清除在裂变期间释放的过量卤素方面有用,但是没有进行具体提议用于控制裂变产物的有害影响。
概述
根据本发明的一个方面,提供了牺牲金属(sacrificial metal)在熔盐裂变燃料的核裂变反应堆中的用途,所述用途为了控制从所述熔盐释放的挥发性碘化合物的水平,其中所述牺牲金属是锆、钒、铬和银中的一种或任意的组合。
根据本发明的另一个方面,提供了一种管理(控制或解决,manage)在裂变反应堆中的气体产生的方法,所述裂变反应堆包括容纳熔盐裂变燃料的燃料管。所述方法包括使所述熔盐连续地与牺牲金属接触,对所述牺牲金属进行选择以便控制从所述熔盐释放的挥发性碘化合物的水平,其中所述牺牲金属是锆、钒、铬和银中的一种或任意的组合。
其他方面在权利要求2及后续等等中提出。
附图简述
现在将通过仅示例的方式并且参照附图来描述一些优选的实施方案,其中:
图1示出了容纳熔融燃料盐的燃料管的实例;
图2a、2b和2c示出了用于允许裂变气体从燃料管排放的三种方法的实例。
详细描述
已经进行了将牺牲金属结合到燃料盐或燃料管中的效果的系统分析,结果是鉴别了用于此目的的特别有效的金属。三个因素决定(支配,dictate)了任何具体牺牲金属的适合性。这些是
·维持低氧化还原态并且因此维持低金属腐蚀能力以及如由熔盐中的三价锕系元素与四价锕系元素的高比率指示的低浓度的锕系元素四卤化物,同时在接近该盐混合物的沸点的温度没有将锕系元素(通常为铀)卤化物还原为金属形式。
·化学地结合熔盐中的潜在挥发性裂变产物并且防止它们进入所述盐上方的气相。特别重要的是将挥发性碘化合物(尤其是TeI2)减到最少。
·将反应性碲转化为稳定的碲化物以防止碲诱发的与所述熔盐接触的金属(尤其是镍合金)的脆化。
已经使用软件程序HSC Chemistry 7进行了这三个因素的热力学计算。结果在表1中示出。
热力学计算的参数为如下。牺牲金属以与其他反应物相比过量的单独的纯金属相提供。
盐组成,以摩尔为单位:
这代表接近其在快速光谱核反应堆中的使用寿命末期的典型燃料盐。已经排除了第1和2族金属、镧系元素、贵金属和稀有气体(惰性气体,noble gasses),因为它们被证实对所涉及的化学没有影响。在600℃确定气体组成并且铀在1500℃还原为金属。
表1的考查表明,在挥发性物种的控制不重要的情况下,锆、钛、铌、钒、锌、铬、银和锰适合作为牺牲金属以控制氧化还原态同时不产生铀金属。
此外,在危险挥发性物种如碘的控制重要的情况下,则仅锆、钛、钒、铬和银是可用的。除钒之外,这些相同的金属在控制碲水平方面也是有效的。
作为牺牲金属,银看起来具有独特的性质。尽管其高的鲍林电负性(Paulingelectronegativity),但是其在降低UCl4浓度、降低挥发性碘物种和清除碲方面非常有效。对碘的高亲和力是银的已知性质,但是在将UCl4还原为UCl3的功效方面是出乎意料的。
在特定的牺牲金属针对以上给出的三个因素更有效的情况下,多种牺牲金属的组合仍然产生更有利的结果。
尽管对于氯盐(chloride salt)已经提供了数据,但可以将相同的原理和可用的牺牲金属应用于氟盐(fluoride salt)体系。
尽管熔盐化学利用牺牲金属的被动控制对于熔盐反应堆来说具有普遍价值,但对于反应堆(如GB 2508537中描述的反应堆)来说是特别重要的,其中接近(进入,access)熔盐以对所述化学的主动控制(例如通过加入少量反应性金属)具有挑战性。在这样的反应堆中,有用的是在熔融燃料盐水平上方或下方将牺牲金属施加至容纳该盐的容器。这防止了牺牲金属被沉积的贵金属裂变产物堵塞。还可以有利的是,尤其是在牺牲金属具有显著的中子吸收的情况下,牺牲金属不位于反应堆芯的中心附近,使得任何中子吸收被最小化。
牺牲金属可以以多种方式提供。图1a至1e示出了结合牺牲金属的燃料管的实例。图1a示出了容纳熔盐103a的燃料管101a和施加至该燃料管的内壁的牺牲金属的内部涂层102a。可以通过多种方法将牺牲金属施加至燃料管的内壁,包括但不限于电镀、等离子体喷雾、浸渍到熔融金属中、硬钎焊、焊接、化学气相沉积、溅射、真空沉积、转化涂布、喷雾、物理涂布和旋涂。备选地,如图1b中所示,可以将内部涂层105b仅涂覆至燃料管101b的一部分,条件是该部分与燃料盐103b接触。图1c示出了另一个实施方案,其中将由牺牲金属制成或涂布有牺牲金属的金属插入物104c放置在燃料管101c内部的熔盐103c内。可以使该插入物成形以辅助燃料盐的对流混合,例如螺旋成形。图1d示出了又一个实施方案,其中牺牲金属作为在燃料管101d内的熔盐103d中悬浮的粒子107d或作为在这样的粒子上的涂层提供。图1e示出了一个实施方案,其中牺牲金属作为被允许在燃料盐103e中下沉至燃料管101e的底部的粒子106e提供。
牺牲金属如钛、钒、铬或银的使用将由燃料盐产生的许多放射性物种的蒸气压(蒸汽压,vapour pressure)降低至非常低的水平。这使得可以用简单得多的方法来管理从燃料释放的气体(在合适牺牲金属存在下,其主要是稀有气体、氙和氪)、镉和锆卤化物,尽管在将锆用作牺牲金属的情况下后者的浓度显著降低。这些气体在燃料元件中的累积是这样的燃料元件的寿命的主要限制,因为如果气体被允许累积,它产生高压力,其可以使燃料元件的覆层破裂。
已知的是,特别是在钠冷却的快速反应堆中,可以允许裂变气体从燃料元件排放到钠冷却剂中。这种做法在开发这样的反应堆的早期使用,但是因为在排放的气体中存在高度放射性的、相对长的半衰期的铯而被放弃。铯污染钠冷却剂并且使得钠的处理极具难度以及在钠火灾事件中产生重大危险。因此中断了这种做法。对于不同于钠冷却反应堆的反应堆,从未提议类似的排放程序。
熔盐反应堆在不积累挥发性金属形式的铯方面是独特的,其作为气体从金属核燃料元件释放并且在陶瓷核燃料元件中的部分泄漏的高压气体微泡中累积。在熔盐反应堆中,铯形成非挥发性卤化铯,其在所涉及的温度下具有可忽略的蒸气压。因此可以将裂变气体从熔盐反应堆排放至冷却剂中,同时不引起严重水平的污染。对于GB 2508537中描述的熔盐反应堆设计来说,这是特别相关的,其中的备选方案是收集气体的相对复杂的管道系统构造。
以这种方式释放的气体仍然含有大量的放射性碘,但是具有短的半衰期。该放射性碘将会污染冷却剂,但是将会在相对较短的时间段内衰减至无害水平。然而,牺牲金属如镁、锆、钪、钛、锰、铝、钒、铬和/或银的包含将挥发性碘的量降低至较低的水平。因此存在的重大优势是将如上所述的牺牲金属的使用与用于燃料管的气体排放系统进行组合。在文献(ORNL-NSIC-37,Fission Product release and transport in liquid metal fastbreeder reactors(液体金属快速增殖反应堆中的裂变产物释放和运输))中描述了适合的气体排放系统并且其包括“潜水钟(diving bell)”装置、窄或毛细管道以及位于燃料盐水平上方的气体可透过烧结物(sinter)。可以将气体排放到冷却剂盐上方的气体空间中或直接排放到冷却剂盐中,在那里其将会鼓泡至表面。
图2a至c示出了允许裂变气体从燃料管排放的三种方法。2a中所示的方法利用燃料管203a的上开口用烧结金属塞(sintered metal plug)201a的封闭,其中调节烧结物孔径以允许气体通过但是不允许液体(无论是燃料盐202a还是燃料管外部的冷却剂)通过。图2b示出了容纳燃料盐202b的燃料管203b,其中燃料管由潜水钟组件205b覆盖。潜水钟组件205b允许气体经由燃料管的壁上的通风口206b从燃料管203b通过至冷却剂207b,但是被吸入到潜水钟组件205b中的冷却剂207b不能与燃料盐202b混合。图2c示出了经由窄管或毛细管208c直接排放至冷却剂207c上方的气体空间的燃料管203c。
Claims (15)
1.熔盐裂变燃料中的牺牲金属在具有所述熔盐裂变燃料的核裂变反应堆中的用途,所述用途为了控制从所述熔盐裂变燃料释放的挥发性碘化合物的水平,其中所述牺牲金属是锆、钒、铬和银中的一种或任意的组合。
2.根据权利要求1的用途,其中所述熔盐裂变燃料包含锕系元素卤化物。
3.一种管理裂变反应堆中的气体产生的方法,所述裂变反应堆包括容纳熔盐裂变燃料的燃料管,所述方法包括使所述熔盐裂变燃料连续地与牺牲金属接触,对所述牺牲金属进行选择以便控制从所述熔盐裂变燃料释放的挥发性碘化合物的水平,其中所述牺牲金属是锆、钒、铬和银中的一种或任意的组合。
4.根据权利要求3的方法,并且包括允许在所述熔盐裂变燃料的裂变期间产生的气体离开所述燃料管而进入在所述燃料管周围的冷却剂中或进入与所述冷却剂接触的气体空间中。
5.根据权利要求3的方法,其中所述牺牲金属作为在所述燃料管中的镀层提供。
6.根据权利要求3的方法,其中所述牺牲金属作为在所述熔盐裂变燃料中的粒子或作为粒子上的涂层提供。
7.根据权利要求3的方法,其中所述牺牲金属作为浸入所述熔盐裂变燃料中的插入物或作为在浸入所述熔盐裂变燃料中的插入物上的涂层提供。
8.根据权利要求3至7中任一项的方法,其中所述熔盐裂变燃料包含锕系元素卤化物。
9.一种用于在核裂变反应堆中使用的燃料管,其中所述燃料管被配置成容纳熔盐裂变燃料,所述燃料管包含牺牲金属,使得在使用中所述牺牲金属与所述熔盐裂变燃料接触,或者与由从所述熔盐裂变燃料形成的蒸气冷凝的液体接触,对所述牺牲金属进行选择以便控制从所述熔盐裂变燃料释放的挥发性碘化合物的水平,其中所述牺牲金属是锆、钛、钒、铬和银中的一种或任意的组合。
10.根据权利要求9的燃料管,其中所述燃料管被配置成允许气体从使用中的所述燃料管离开而进入包括所述燃料管的裂变反应堆的冷却剂或气体空间中。
11.根据权利要求10的燃料管,其中所述燃料管的开口用烧结塞封闭,所述烧结塞被配置成允许气体通过而不允许液体通过。
12.根据权利要求10的燃料管,所述燃料管在使用时垂直地延伸到所述气体空间中,并且包括在所述气体空间内的开口。
13.根据权利要求12的燃料管,其中所述燃料管包括在使用时垂直地延伸到所述气体空间中的毛细管,并且所述开口在所述毛细管的上端处。
14.根据权利要求9的燃料管,其中所述牺牲金属作为在所述燃料管的表面上的镀层提供。
15.根据权利要求9的燃料管,其中所述牺牲金属作为在所述燃料管中的粒子或作为粒子上的涂层提供。
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