CN102985357A - 用于处理含氚气体的膜反应器 - Google Patents
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Abstract
一种用于通过同位素-交换工艺从污染的气体混合物回收氚的设备,其特征在于其包含具有优选圆柱形状的由钢或其它适合的金属或玻璃制成的容器,称为“组件”(1),其含有至少一个由可选择性渗透氢及其同位素的金属或金属合金制成的渗透器管(T),其中所述管(T)以悬臂方式设置,其自由端是封闭的,进一步地提供用于在所述渗透器管(T)的自由端上施加轴向张力的装置和用于所述管(T)的自由端到相邻的组件(1)的端部法兰(FF)的电连接的装置。
Description
技术领域
本发明所述装置基本上由膜反应器构成,所述膜反应器使用了由钯银合金制成的管(渗透器管),其具有选择性地渗透氢及其同位素的性质。所述装置被设计用于实施从来自实验室和工厂的材料(所谓的“软性家务废物”,即,手套、纸张等)中回收氚的新工艺,其中,被氚污染的材料被处理。
在这里描述的膜反应器中,在来自“软性家务废物”除氚工艺的氚化气体流与冲洗氢气流之间以逆流进行同位素交换。本发明设想在基本构造中采用一端封闭的由钯合金制成的管(按照“指状”或“套管”设计)和由电流流通的焦耳效应而产生的热。特别地,提供了如下装置,其配备有能够同时在渗透器管上施加拉伸应力并且能够使电流流过以用于所述渗透器管本身的欧姆加热的装置。
从下面的详细说明并参考附图(其纯粹是对非限制性实施例和其优选的实施方案的图示)将会对本发明有更好的理解。
在所述附图中:
图1-4显示了根据现有技术的设备;
图5是根据本发明的一种膜反应器的纵向剖视图;
图6与前一幅相似,显示了一种变体,其在端部法兰上具有绝缘的电通路;
图7和8,其分别与前面的图5和6相似,是关于本发明的第二种实施方案,其设计了用于调节由弹簧施加到渗透器管上的张力的装置;并且
图9和10显示了本发明所述反应器的两个附图,分别用于端部法兰通过电绝缘衬垫连接的情况和使用绝缘电通路的情况。
1、所属领域状态
为了在核-热核反应堆的燃料循环研究应用[1,2]中从气体流中去除氚,已经提出了使用由钯银合金制成的渗透器管的膜反应器(PERMCAT)。在所述已知反应器的第一构造中,把氢气流送入可选择性渗透氢同位素的由钯银合金制成的管状膜,其中所述氢气流相对于含有氚和氚标记化合物(例如,氚化水和甲烷,此外还有CO、CO2以及惰性物质)的气体流是逆流的,其被送到位于反应器本身的壳体中的催化床层之上,如图1所示,其中氚由字母Q所指示。
所使用的Pd-Ag渗透器管具有0.100mm厚度的壁,其特征为高的长度-直径比(外径3.3mm和长度500mm)。通常,使用由钯合金制成的管的这种膜反应器存在与热循环和氢化/脱氢循环相关的缺点,其涉及到所述管本身的延长/收缩。如果所述变形被反应器组件阻止或妨碍,可以产生机械应力,包括环状的应力,会引起所述膜的迅速损坏,同时造成选择性的损失,并因此引起所述装置功能的损失。为了克服这些缺点,ENEA在过去研究了膜反应器的特别构造,在其中使用了薄壁的(0.050mm)渗透器管,其特征为更高的氢同位素渗透流量[3]。在该构造中,钯管通过两个金属伸缩软管以液密的方式被连接到反应器组件,所述金属伸缩软管能够补偿不同的变形并且此外,在安装步骤期间,通过拉伸所述金属伸缩软管焊接到反应器组件将钯管固定,并使用伸缩调整器将所述金属伸缩软管相对于其静止位置而方便地伸长(图2)。用这种方法,在操作条件下,所述管状膜受到与材料的构造和特征相适应的轴向拉伸应力。但是,由于与催化床层接触时的磨损或腐蚀,小的壁厚(0.050mm)可以导致缺损(小孔或裂纹)的形成。
在其它已知的应用中,例如同时用于除氚工艺和脱氢反应两者,已经研究了其中渗透器管仅仅在一端固定到反应器组件上的膜反应器;该构造被称为″指状″或″套管″构造。事实上,所述渗透器管在其一端是封闭的,同时一根较小的管***到其内腔中,作为供应或回收保留物的入口。例如,如图3所示的是膜组件的示意图,所述膜组件使用了指状构造的Pd-Ag渗透器管:透过所述膜的氢气由冲洗气体收集在反应器的壳中,同时通过***所述渗透器管内腔的小直径钢管而回收保留物(非透过气体)。
但是,这些已知的构造,特别是在渗透器管很长的情况中(即,其中要求高的除氚因子),存在渗透器管T与膜组件1的内壁接触和干扰的缺点,这是由于热循环和加氢循环所导致的管T本身所经历的变形而造成的。关于这一点,应参考图4,其中显示了在热循环和加氢循环的耐久试验前后由Pd-Ag合金制成的渗透器管。
最后,为了降低所需的电能并防止不必要的热工艺气体流,最近已经提出了由钯合金制成的欧姆加热渗透器管[4]。但是,这些装置要求通过所述反应器组件壁的特别的电通道,以及足够的用于渗透器管至电通道本身的柔性连接的***。
本发明的主要目的是通过提供如所附权利要求1所描述的膜反应器来克服上述的问题,其中设计了基本上圆柱形的容器,其被称为“组件”1,其优选由钢制成,但还可以由其它金属和其它材料制成:例如,对于实验室应用,玻璃(例如,硼硅酸耐热玻璃Pyrex)经常是优选的。
2、本发明概述
构成本发明主题的膜反应器包含至少一个由钯银合金制成渗透器管T(优选地具有23-25wt%的Ag),其壁厚为大约0.050mm-0.200mm。在管壁厚为大约0.050mm情况下,这些是由轧制和随后扩散焊接生产的薄壁管[5];在管壁厚为大约0.200mm情况下,这些是市售可得的管,其从大约100μm的厚度开始。
应当注意通常被用作渗透器管的合金是钯基合金,例如PdCu,但基于Ni、Nb、V、Ta、Ti也在研究之中。如前面所提到的,用于所述致密金属管状膜的实际厚度基本上包含在50-200μm的范围内。
所述渗透器管T被容纳在指状构造的组件1中,其中被送入内腔以及被送入外壳的两气体流以逆流运行。通过电流通路来实现直接欧姆加热,而将管T加热到大约等于300-400℃的工艺温度。
根据本发明的特别的特征,提供了一种应用于渗透器管T封闭端的特别装置,其基本上由优选的双金属弹簧M组成,所述双金属弹簧M具有两个非常不同的功能:
-向所述渗透器管T施加能够防止与所述膜组件1内壁接触和干扰的拉伸负荷,所述接触和干扰是因为渗透器管T经受由热循环和脱氢循环而导致的变形;和
-保证在渗透器管T的封闭自由端与膜组件1的外部之间的电连接,从而能够通过所述管本身的焦耳效应来加热。
在这里描述的示例性实施方式中,为了提供机械张力和电连接装置,已经研究了弹簧M的构造:
能够保证电流通路的银线,其具有低电阻从而防止弹簧M本身的加热并且限制由于渗透器管T上的欧姆效应而导致的加热。
特别地,银的机械刚度可以被认为是微不足道的。同样地,由于银线具有大得多的电导率,其特征为更低的电阻率和适当地大于Inconel线的横截面,通过所述Inconel的电流通路(以及相应的由焦耳效应而发生的加热)是无关紧要的。
图5和6是本发明的示意图,其中突出显示了两个变体的双金属弹簧M的细节:
a)通过使用法兰本身的密封垫圈(其由绝缘有机材料(硅氧烷、Viton、Vespel等)制成)和也是由绝缘材料制成的特别的衬套(其用于紧固所述法兰的螺栓),实现对膜组件1的端部法兰FF的电绝缘(图5);和
b)使用穿过膜组件1的端部法兰FF的绝缘电通路(图6)。
本发明的第二种实施方案,如图7和8所示,设计了用于调节由弹簧M施加到渗透器管T上的张力的装置。
在这里还图示了端部法兰的电绝缘(图7)和绝缘电通路的使用(图8)的两个案例。更具体地说,通过特意提供的调节杆的动作来调节由弹簧M施加的张力,所述调节杆最后以通过直接焊接-钎焊到端部法兰(图7)或者绝缘电通路(图8)的密封方式而被阻挡。
2.1双金属的弹簧的尺寸
对于所述试验,双金属的弹簧M的尺寸是基于渗透器管T在操作条件下在大约300-400℃的温度范围内的机械特性(屈服点)和电特性(电阻率)而制定的。特别地,例如,对于10mm直径的所述Pd-Ag管,要考虑不同的壁厚(0.050和0.200mm)和长度(250和500mm)值。
为了防止所述渗透器管在300-400℃的工作温度的任何过度变形(也被称为“蠕变”现象),要施加的拉伸负荷被固定为400℃温度下极限抗拉强度(UTS)的大约5%。由文献[6、7]所提供的数据,Pd-Ag合金(23-25wt%Ag)的计算UTS值是280MPa。因此,对于具有0.050和0.200mm壁厚的渗透器管,弹簧M施加到管T的拉伸负荷值(其被计算为所述UTS的大约5%)分别为20和80N。
在现有工作[8]已考虑的温度范围内和加氢条件下,Pd-Ag管长度变化百分比估计为大约1.5%,因此对于总长250mm的渗透器管来说,相应的长度绝对变化为大约4mm,而对于长度为500mm的管T来说,相应的长度绝对变化为大约8mm。
表I中是所述双金属弹簧M的Inconel部分的尺寸。匝数以如下的方式来计算:在工作条件下弹簧M长度的变化(“匝数”ד偏移”)比所述渗透器管T长度的绝对变化(作为热循环和加氢循环的结果)大10倍。用这种方法,可以合理地发现随渗透器管T的伸长/收缩而由弹簧M施加的张力负荷的变化基本上是微不足道的(即,是最初施加负荷的大约10%)。
表I
考虑到所述银线具有与所述Inconel线相同的长度(即,所述银线和Inconel线被收卷在单个的线圈内以形成双金属弹簧),确定了所述双金属的弹簧M中银部分(其用于实现具有尽可能低的电阻的导电)的尺寸。此外应当考虑所述银部分的电阻要比所述渗透器管T的电阻足够地低:特别地,银线的电阻被固定为Pd-Ag管T电阻的10%,其是假设所述合金的电阻值为4x10-7Ωm来计算的。计算的Ag线的直径值当渗透器管T壁厚为0.050时大约为Ψ=1.5mm,且当渗透器管T壁厚为0.200mm时Ψ=3mm(见表II)。
表II
反应器的实例
对于有关JET(欧洲联合环形加速器)的除氚***应用,反应器组件1被设计包含长度250mm,直径10mm,且壁厚0.050mm的Pd-Ag渗透器管T。在这种情况下,所述双金属弹簧M被构造为20匝直径1mm的Inconel线和厚度1.5mm的银线。图9和10代表了所述组件1的两个附图,分别对应于端部法兰通过电绝缘衬垫连接的情况(图9)和使用绝缘的电通路的情况(图10)。在两种情况下都设计使用用于调节张力的***,其通过特意提供的杆构成,根据情况,所述杆在安装操作结束时以密封方式(焊接-钎焊、惰性气体保护钨极焊等)而被直接固定到法兰FF末端,或者借助于绝缘的电通路而固定。
所述组件1还被设计使用热电偶用于探测在所述渗透器管中心部分附近的温度。
应当注意在这里描述的双金属弹簧M是一种可以以不同的方法实施的对象,条件是保证其双重功能,即,张力的施加和电的传导。
例如,除可能由收卷在同一个线圈中的两个单独的金属线(Inconel线和银线)制成之外,还可以通过提供两个不同的共轴弹簧,它们具有不同的直径不同的螺距等,且一个在另一个内部来加以实施,或者它可以构造为由特殊材料所制成的单个弹簧M,所述特殊材料在所指出的工作温度下兼具所要求的机械抗力和高的电导率特征。
应当注意上面描述的优选双金属的弹簧M是很重要的,其是为了保证所述渗透器管T的变形(随热循环和加氢循环的伸长和收缩)通过施加适当的张力而在轴向被引导。
应当注意这些装置(即,使用了由Pd-Ag合金制成的渗透器管T的膜反应器)的特别应用要求在所述Pd-Ag管T外部与所述膜组件1壳的内部之间具有很小的环隙,其中所述渗透器管是指状构造的,即,设置为悬臂的方式且其自由端封闭。事实上,这些装置运行效能的高水平用术语除氚因子来表示,即,输入和输出气体中氚浓度的比率,所述运行效能的高水平不仅显著地依赖于在催化床上发生的同位素交换反应的动力学,还依赖于主要通过所述管状膜壁和通过不同的气体薄膜的氢同位素渗透的动力学。
渗透的动力学反过来由对氢同位素材料传输的阻力来决定:在这种意义上讲,在所述渗透器管和组件壳之间的环隙的大厚度气体层的存在导致氢同位素的浓度梯度,其引起了对传输的阻力。
因此,为了得到高的除杂因子,恰恰需要尽可能地降低所述渗透器管T和组件1的壳之间的环隙。但是,在指状构造的情况下,并且由于热和脱氢循环,小尺寸的环隙可以引起渗透器管与膜组件1的内壁的接触和干扰。为此,对于根据本发明除氚工艺的专门应用并且更一般而言对于所有那些其中要求高动力学渗透的情况,一种能够以轴向方式引导所述渗透器管T的变形的***提供了特别的优越性,这是通过在所述渗透器管上施加足够的张力而得到的。
3、应用
形成本发明所述主题的装置已经被特别地设计用于来自加热室的气体流的除氚,所述加热室用于处理所谓的实验室“软性家务废物”即,手套、纸张等)。
更一般而言,本发明可被用于磁约束试验机(例如JET和ITER-国际热核实验性反应堆)的等离子体排放物的处理,或者用于所有使用由Pd-Ag合金制成的管状膜来分离气相氢同位素(H、D、T)的工艺,例如,气体流的净化(除氚)、同位素分离或富集工艺等。
但是,考虑到潜在的市场,最重要的应用是关于生产用于氢气净化的膜组件和用于通过脱氢反应生产超高纯度氢气的膜反应器。除了那些生产用于实验室使用的超高纯氢气的装置之外,这些应用可以针对那些在化学工业的特别领域(精细化学、药物领域)使用聚合类型燃料电池(PEM燃料电池)的***。
在所述不同的应用中,可以证明改变目前所描述对象的尺度(长度、直径、催化剂的类型和容量等)是必需的,同时也要提供含有许多渗透器管T的装置或提供许多串联或并行的膜组件1的组合。
最后,可以设想冲洗所述气体流的不同方式。
总之,用于供给所述膜的流(H2)可以通过小直径的钢管输送,并且保留物(富Q2流)的回收可以通过所述渗透器管来实施。同样送入内腔的流可以与送入所述组件壳的流相交换(即,H2/Q2流被送入反应器壳并且流CH4+CO+CO2+H2+H2O/CQ+CO+CO2+Q2+Q2O被送入渗透器管的内腔)。
此外,所述送入内腔并送入壳之中的气体流可以以逆流方式运行,或者以等同流(equicurrent)方式运行(即,以相同的方向横穿所述反应器)。
最后,可以设想所述渗透器管T内部或外部的催化剂的使用和位置。
4、参考文献
[1]M.Glugla,A.Perevezentsev,D.Niyongabo,R.D.Penzhorn,A.Bell,P.Hermann,APERMCAT Reactor for Impurity Processing in the JET Active Gas Handling System,Fusion Engineering and Design 49-50(2000)817-823
[2]B.Bornschein,M.Glugla,K.Gunther,R.Lasser,T.L.Le,K.H.Simon,S.elte,Tritiumtests with a technical Permcat for final clean-up of ITER exhaust gases.FusionEngineering and Design 69(2003)51-56
[3]S.Tosti,L.Bettinali,F.Marini,Dispositivo per la rimozione di trizio da correnti gassose,Italian Patent n.RM2005U000165(14.12.2005)
[4]S.Tosti,L.Bettinali,R.Borelli,D.Lecci,F.Marini,Dispositivo a membrana dipermeazione per la purificazione di idrogeno,Italian Patent n.RM2009U000143(15.09.2009)
[5]S.Tosti,L.Bettinali,D.Lecci,F.Marini,V.Violante,Method of bonding thin foils madeof metal alloys selectively permeable to hydrogen,particularly providing membranedevices,and apparatus for carrying out the same,European Patent EP 1184125 A1
[6]ASM Handbook,vol.2,Properties and Selection:Nonferrous Alloys andSpecial-Purpose Materials,ASM International 1990,ISBN 0-87170-378-5(v.2)
[7]http://www.platinummetalsreview.com
[8]S.Tosti,L.Bettinali,F.Borgognoni,D.K.Murdoch,Mechanical design of a PERMCATreactor module,Fusion Engineering and Design 82(2007)
Claims (7)
1.一种用于通过同位素交换工艺从污染的气体混合物回收氚的设备,其特征为所述设备包含优选圆柱形的由钢或其它适合的金属或玻璃制成的容器,称为“组件”(1),其含有至少一个由可选择性渗透氢及其同位素的金属或金属合金制成的渗透器管(T),其中所述管(T)以悬臂方式设置,其自由端是封闭的;进一步地提供用于在所述渗透器管(T)的自由端上施加轴向张力的装置和用于所述管(T)本身的自由端到相邻组件(1)的端部法兰(FF)的电连接的装置。
2.根据权利要求1所述的设备,其特征为:
-所述组件(1)在其两端通过密封法兰而封闭;
-所述管(T)由Pd-Ag合金制成并且通过钎焊或焊接到所述组件的第一法兰而被固定;
-所述渗透器管(T)在一端封闭,并且通过设置在所述渗透器本身内腔的,由钢或其它适合材料制成的指状构造的另外的小直径管而进行保留物的回收;
-所述由Pd-Ag制成的渗透器管(T)的封闭端通过弹簧(M)连接到组件(1)的第二法兰(FF),所述弹簧(M)被设计成能施加轴向张力并提供电流通路;和
-通过由电绝缘材料制成的衬垫以及由电绝缘材料制成用于螺栓的衬套而将所述第二法兰(FF)固定到组件上,所述螺栓用于紧固所述法兰。
3.根据权利要求1所述的设备,其特征为所述用于施加轴向张力并提供电流通路的装置是由通过绝缘的电通路连接到第二端部法兰(FF)的弹簧(M)而构成,所述法兰具有金属衬垫并且不要求具有由电绝缘材料制成的衬套。
4.根据权利要求2或权利要求3所述的设备,其特征为它还包括用于调节由弹簧(M)所施加张力的装置,该装置具有调节杆,其设计成能通过钎焊焊接以密封方式来被阻挡。
5.根据权利要求1所述的设备,其特征为所述渗透器管(T)由Pd-Ag金属合金制成的管组成。
7.根据权利要求1所述的设备,其特征为所述用于施加轴向张力并提供电流通路的装置是这样构造的:
通过卷绕在同一螺旋上的两条不同材料的线而得到的弹簧(M);或者是
两个共轴的不同的弹簧:一个用于施加张力,并且另一个用于建立低电阻的电连接。
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Also Published As
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RU2558888C2 (ru) | 2015-08-10 |
CN102985357B (zh) | 2015-06-10 |
EP2582618B1 (en) | 2014-05-14 |
ES2494265T3 (es) | 2014-09-15 |
ITRM20100330A1 (it) | 2011-12-17 |
JP5798187B2 (ja) | 2015-10-21 |
CA2802208A1 (en) | 2011-12-22 |
CA2802208C (en) | 2017-10-31 |
WO2011158275A8 (en) | 2013-01-10 |
KR20130129823A (ko) | 2013-11-29 |
IT1401192B1 (it) | 2013-07-12 |
US20130108517A1 (en) | 2013-05-02 |
KR101736530B1 (ko) | 2017-05-16 |
RU2013100180A (ru) | 2014-07-27 |
EP2582618A1 (en) | 2013-04-24 |
JP2013536404A (ja) | 2013-09-19 |
US8979984B2 (en) | 2015-03-17 |
WO2011158275A1 (en) | 2011-12-22 |
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