CN103890858A - 捕集通过密闭空间内的辐解或热解产生的可燃气体的设备 - Google Patents

捕集通过密闭空间内的辐解或热解产生的可燃气体的设备 Download PDF

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CN103890858A
CN103890858A CN201280005418.0A CN201280005418A CN103890858A CN 103890858 A CN103890858 A CN 103890858A CN 201280005418 A CN201280005418 A CN 201280005418A CN 103890858 A CN103890858 A CN 103890858A
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瓦伦廷·罗尔
伊利萨·莱奥尼
乔斯林·普里让
米歇尔·拉特罗切
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Abstract

一种用于捕集诸如氢气之类的可燃气体的设备，包括壳体（1）内的活性剂装置（3），所述壳体除了被过滤器（2）堵住的开口外均封闭，所述过滤器通常只允许要捕集的气体穿过过滤器。捕集在壳体内维持减小的压强，所述减小的压强持续地将外部产生的气体吸入。捕集器能够在没有任何维护的情况下进行操作并且持续很长一段时间，甚至是在完全密闭的环境中。

Description

捕集通过密闭空间内的辐解或热解产生的可燃气体的设备
技术领域
本发明的主题是一种用于捕集通过密闭空间内的辐解或热解或者辐解和热解两者产生的可燃气体的设备，所述容积形成于用于运输和/或储存放射性物质的罐体或者其它系统中。通常由这些现象产生的这样的气体是氢气。
背景技术
核设施引发一定数量的“技术废料”，所述技术废料可以包括具有非常多样的性质的物体和材料（例如，过滤器、金属废料、碎石、玻璃等），或者反而是基于有机材料的纤维素（例如，纸张、木头、棉、或诸如由乙烯基或聚氨酯制成的包装罩的塑料材料、靴子、手套以及被认为是聚合物的材料制成的各种物体）。所有这些废料还能够污染少量的液体（例如，水）和有机液体（例如，油或者碳氢化合物）。全部废料组成在处于核设施中期间被激活或者在用于所述设施中期间被包括铀或钚的放射性元素的粉尘污染的材料，所述放射性元素能够发射α、β、γ粒子等。
这些技术废料的运输和储存造成了与被运输材料的性质相关的特定的困难。事实上，如之前所述，这些废料被包括铀或钚的放射性元素污染，放射性元素给予废料放射性特性。在由放射性元素产生的辐射作用下，组成废料的材料能够衰变并且释放气态的化合物，其中某些是可燃的。产生的气体为氢气、一氧化碳和二氧化碳、氧气、氮气以及挥发性有机化合物（VOC）。这一现象称为辐解。当技术废料被限制在缩小了体积的密闭容器中时，因为可燃气体的产物在没有排出的可能的情况下能够快速达到高浓度，所以这样的可燃气体的产物造成了问题。在氢气的情况下，空气中的可燃性阈值在4%附近。当浓度超过这一阈值时，热源或者火星足以点燃气态的混合物或者产生剧烈的爆燃。
各种研究和观察已经示出了，随着技术废料放射强烈的α粒子并且包含大量的有机分子时，可燃气体（例如，通过在含有具有氢化化合物的放射性材料的密闭容器中的辐解产生的氢气）的浓度有时能够在几天之后达到4%附近的值。
现有技术包括各种用于（特别是通过催化氧化）捕集诸如氢气之类的可燃气体的设备，所述催化氧化使得氧气和氢气重新结合形成水。
专利FR-A-2874120描述了这样的添加有第二催化剂的催化剂在密闭容器中的使用，由于CO是氢气的氧化反应中的抑制剂，所述第二催化剂激发另一将CO转化为CO2的氧化反应。第一催化剂有利地为灌注有钯的氧化铝的形式，第二催化剂为包括CuO和MnO2的混合物的形式。
这些通过氧化的化合物的缺点是只有覆盖空气含有足够量的氧气才起作用，由于有机物质（尤其是碳链）的辐解并不产生氧气以及相反地存在的氧气可能被有机物质的氧化反应消耗，所以并不总是存在足够量的氧气。
专利FR-A-2925752描述了一种能够在密闭容器中进行受控的氧气释放的设备，以解决这一困难；但是该解决方案依然很难变得很可靠。
其它捕集器包括在不使用氧气的情况下捕集可燃气体的金属氢化物或金属氧化物，被称为活性剂装置或“吸气剂”。这些活性剂装置（active means）可以是可逆的（金属氢化物的情况）或者不可逆的（金属氧化物的情况）。在第一种情况下，可燃气体可以在特定的压强和温度条件下被释放。不过，所述活性剂装置的缺点是存在抑制剂气体（尤其是CO）存在下其效率大幅减小。但是，在几乎全部情况下，聚合物废物的热化学和辐解的衰变导致这些抑制剂的大的浓度。
申请文件US-A-6262328和WO-A-2010/066811相继描述了覆盖在多孔基体中的活性剂装置，该具有在使有害物停止的同时对混合物进行过滤并且同样地使得被捕集的气体到达活性剂装置的能力。这样的基体可以是能够透过氢气的玻璃基体、接合剂基体或者沸石。然而，因为很难使基体中的活性剂装置的分布最优化以使能有效的捕集，必须承受一定程度的效率缺乏：因此大量的活性产物是必须的。另外，如果活性产物不再满足，特别是如果活性产物饱和，那么不可能只替换活性产物，基体也必须要被替换。
过滤设备进一步基于多微孔膜或其它而存在，但是因为并不关系到被限制的容器并且是基于气流或者压差的形成以迫使流过膜，则多微孔膜与本发明的条件无关。例如，可以援引申请文件EP-A-0383153，其中催化剂产物被布置为穿过壳体的其中产生氢气的开口：催化剂被包裹在被提供有在出口处的网格以及悬置的过滤器的外壳中，然而，在壳体的侧面，所述外壳对于混合物的所有气体来说都是能透过的；壳体中的超压气体因此在流出之前穿过过滤器和催化剂，氢气在此通过产生水的重新结合被消除。
申请文件EP-A-0670575描述了另一设备，其中，催化剂放置在外壳内，外壳除了对过滤器之外都是封闭的。然而，所述设备并没有解决催化剂中毒的问题，以至于催化剂保持与气体产物媒介隔离，直到氢气的侵入变得明显。催化剂随之暴露于该媒介。监视的必要性以及捕集操作或者当捕集开始活化时的机制是相当长的持续时间的过程的主要缺点，在此持续时间中氢气的出现是不可预料的，或者完全相反地为缓慢且规律的，这将使得捕集总是活性的以避免其积累。过滤器似乎并不对气体施加任何选择效果并且是简单的颗粒过滤器（HEPA）。不能确定的是，如果捕集被短时间活化而非永久活化，则能够获得高效率。
发明内容
本发明的基本理念在于在罐体的其中发生辐解和/或热解的密闭空间中引入一箱体，所述箱体的至少一面装备有混合物的选择性过滤器以允许可燃气体尤其是氢气穿过。用于捕集氢气的活性产物被放置于箱体中并且由此通过过滤器与气态抑制剂（poison）隔离。如果过滤是完美的，那么箱体的内容物理想地由纯可燃气体组成。过滤器具有使混合物的其它气体中的至少一些停止或减缓，并且尤其使为催化反应的抑制剂的一氧化碳停止，以及由于可燃气随着穿透进入箱体中而被捕集，在箱体的内部和外部之间产生局部的压强梯度。由此获得系统，其中存在在密闭空间中的氢气随着一方面形成另一方面被捕集而通过局部压强梯度被导入到箱体中，然而抑制剂气体并不穿透或者非常难以穿透进入箱体。在描述的其余部分里，“箱体”也被称为“壳体”。
因此，本发明的一个方面是一种用于捕集可燃气体尤其是氢气（以及其同位素形式，也就是氘、氚或替代的氘和氚的混合形式）的设备，所述可燃气体通过在用于运输和/或储存放射性物质的系统（所述系统能够是废料罐体、辐射燃料的容器、或者其它）中形成的密闭空间（containment）中的辐解和/或热解而产生，所述设备包括界定一空腔的壳体，能够捕集所述可燃气体的活性剂装置位于所述空腔中，所述壳体除了至少一个被过滤器占据并且仅与所述密闭空间相连通的开口之外是连续的，所述过滤器允许所述可燃气体穿过，其特点是，所述过滤器使其它气体减缓或停止，尤其是使一氧化碳停止。
活性剂装置可以由金属氢化物或金属氧化物组成；它们可在壳体中处于分离且自由的状态，或者被布置为壳体内的板的表面覆盖层，这就保证了活性剂装置是易达到的，特别是与活性剂装置被覆盖在基体中的设备不同，当活性剂装置饱和时能够被替换。
过滤器可以由多微孔层组成，随后过滤根据空间排斥的过程进行，这就抑制或者延迟了大尺寸分子的扩散并且有利于最小尺寸分子的扩散。因为可燃气体相较于抑制剂气体的分子包括更小尺寸的分子，所以多微孔层中抑制剂气体的扩散被大幅度延迟或者甚至是停止，然而恰恰相反，有利于可燃气体的扩散。
过滤器可以由位于主过滤器下的金属膜来完成并且主过滤器完成过滤器；由于过滤的化学方式，通过膜的过滤只允许可燃气体穿过并且使所有其它气体停止。之后根据在膜的表面上的可燃气体的吸收、分解、通过膜的扩散、重新组合以及吸收来实施过滤。在穿过金属膜的整个厚度之后，由此可燃气体出现在壳体中。
由于过滤器对特定气体进行阻止，过滤器保持其所有功用，所述特定气体（其中，又有一氧化碳）通过中毒来妨碍金属膜的正确操作。
过滤器通常包括不具有特别的过滤特性但是确保其机械强度的多孔基质。
多微孔层可以由二氧化硅组成，金属膜能够由钯、钯镍合金、钯银合金、钯铜合金、或钒钨合金和钒镍合金制成。
如果过滤器的选择性被认为不充分，壳体可以进一步包含用于捕集活性剂装置的特定抑制剂的产物（例如，碳酸盐）。
附图说明
参考以下附图将完全以说明的方式来描述本发明：
图1为本发明的一个实施例的全视图；
图2表示本发明的另一实施例；
图3、图4和图5示出布置本发明的两种具体的方式；以及
图6示出过滤器。
具体实施方式
本发明（图1）具有由包括至少一个开口的壳体（1）所界定的箱体的形状，每个开口都由过滤器（2）塞住。壳体（1）包含用于捕集氢气的活性剂装置（3）以及朝着过滤器（2）开口的未被占据的容积（4）。箱体被典型地放置在密闭空间中，密闭空间中的内容物（图中未示出）经受辐解或热解，所述辐解或热解恒定地产生氢气以及对活性剂装置的正确操作有害的抑制剂气体（例如，CO、HCl或HF）。活性剂装置可以是诸如ZrCO或Zr2Fe之类的金属氢化物或者是金属氧化物。在其它安排中，它们可能以自由并且分离的状态在箱体的底部或者，如图2中所表示的悬挂在壳体（1）之中的单独的平板（5）的覆盖层。在此实施例中，壳体（1）包括两个开口并由此包括一对堵住开口的过滤器（2）。
箱体可以被放置在任何地方，例如（图3）在通过上盖（6）闭合的容器形式的罐体（7）的密闭空间（9）内；壳体尤其可以被悬挂在盖子（6）下面，过滤器（2）在壳体的顶部朝着密闭空间（9）的内部容积打开；形成的氢气趋于上升并且被导向箱体，在箱体处氢气被捕获。
然而，在不改变本发明的精神下能够想到其他的安排，例如图4所表现的，其中箱体被放置于罐体（7）的盖子（6）中；含有活性剂装置（3）的箱体（8）随后朝着罐体（7）的内部打开，穿过过滤器（2）并且穿过小的连续的盖子（10）通道外面，所述盖子通过密封件（15）密封，但是可以被移除以替换活性剂装置（3）。图5中表示的另一种可能，包括当通过导管（16）将箱体的内部与罐体外部相连时将箱体放置于罐体（7）的外部；导管（16）以及箱体（1）的开口重合，以使得过滤器（2）还堵住导管（16）。
现在，我们将转向对过滤器（2）的描述。典型地，过滤器包括，如图6示出的从箱体的外部到内部，确保其硬度并能够为金属熔块或由陶瓷制成的多孔基质（11），使得能够阻止特定抑制剂的多微孔层（13）以及用于可燃气体的过滤的金属膜（12），多微孔层（13）随后位于金属膜（12）与更加朝向过滤器（2）的外部的基质（11）之间。除了别的之外，金属膜（12）可以基于钯，所述钯具有根据之前所描述的过程通过化学工具来进行氢气的过滤的能力。随后，氢气根据这一过程穿过金属膜（12）。其中一些已经提过的其它金属合金具有类似的过滤特性。
多微孔层（13）意在保护钯，或者更加一般地保护金属膜（12），同时使能够使金属膜中毒的气体（例如，CO）停止或减缓；多微孔层可以由二氧化硅制成。如所描述的组合了金属膜和多微孔层的复合过滤器可以通过钯在二氧化硅层上的沉积来实现，整体由多孔基质来支撑。
根据第二实施例，过滤器（2）由多孔基质和多微孔层（13）组成，过滤器根据之前所描述的空间排斥的过程通过纯粹地分子过滤来工作。然而，多微孔层对于诸如抑制剂气体（像是，HCl）之类的特定的小尺寸的气体或分子来说是可以透过的。于是这些气体能够进入壳体（1）并且干扰活性剂装置（3）的正确操作。额外的捕集器（14）可以被加入到壳体（1）中以固定（fix）这些气体；不过在特定环境下，可能选择将它们放置于壳体外部。对于上述的气体，令人感兴趣的捕集材料是碳酸盐。同样可以将干燥剂添加到壳体（1）。

Claims (10)

1.一种用于捕集可燃气体的设备，所述可燃气体通过在用于运输和/或储存放射性物质的系统（7）中形成的密闭空间中的辐解和/或热解而产生，所述设备包括界定一空腔的壳体（1），能够捕集所述可燃气体的活性剂装置（3）位于所述空腔中，所述壳体除了至少一个被过滤器占据并且仅与所述密闭空间相连通的开口之外是连续的，所述过滤器（2）允许所述可燃气体穿过，其特征在于，所述过滤器使其它气体减缓或停止，尤其是使一氧化碳停止。
2.根据权利要求1所述的用于捕集气体的设备，其特征在于，所述设备包括，在所述壳体中且置于所述开口上的金属膜（12），所述金属膜（12）实施只允许所述可燃气体通过并且置于所述过滤器与所述活性剂装置之间的过滤。
3.根据权利要求1所述的用于捕集气体的设备，其特征在于，所述设备包括，在所述壳体中的捕集器（14），以对已经穿过所述过滤器（2）的具有小尺寸分子的气体进行固定。
4.根据权利要求3所述的用于捕集气体的设备，其特征在于，所述捕集器由碳酸盐组成。
5.根据权利要求1至4中任一项所述的用于捕集气体的设备，其特征在于，所述过滤器由多微孔层（13）组成。
6.根据权利要求5所述的用于捕集气体的设备，其特征在于，所述多微孔层（13）由二氧化硅组成。
7.根据权利要求1至6中任一项所述的用于捕集气体的设备，其特征在于，所述过滤器包括多孔基质（11）。
8.根据权利要求1至7中任一项所述的用于捕集气体的设备，其特征在于，所述活性剂装置由金属氢化物或金属氧化物组成。
9.根据权利要求1至到8中任一项所述的用于捕集气体的设备，其特征在于，所述活性剂装置在所述壳体中处于分离且自由的状态。
10.根据权利要求1至8中任一项所述的用于捕集气体的设备，其特征在于，所述活性剂装置被布置为所述壳体内的板（5）的表面覆盖层。
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