CN1206458A - 用于热催化床的带通道的陶瓷填料 - Google Patents

用于热催化床的带通道的陶瓷填料 Download PDF

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CN1206458A
CN1206458A CN96199425A CN96199425A CN1206458A CN 1206458 A CN1206458 A CN 1206458A CN 96199425 A CN96199425 A CN 96199425A CN 96199425 A CN96199425 A CN 96199425A CN 1206458 A CN1206458 A CN 1206458A
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plate
rib
unit
ceramic
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CN1144019C (zh
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寇·C·兰格
黄晙
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Lantec Products Inc
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Abstract

陶瓷填料单元(500)由一垛有平行肋(504)且在肋间形成槽的陶瓷板(502)组成。借助与对置板的表面接触把这些槽变成通道。肋(504)可以与毗邻板上的肋端面衔接或者与对置板的肋(504)错开以形成更好的通道。借助烧制成垛的原始状态的板(502)或用无机粘接剂(如硅酸钠)粘接烧结板(502)使多块板(502)彼此结合起来。借助扩大通道的入口(542)或在肋间的板上打孔,可以减少压力降和破裂和提高传质效率和热效率。通过在往塔里放之前在单元组合件周围缠上金属带可以将多个单元预先装配成更大的单元。

Description

用于热催化床的带通道的陶瓷填料
相关的专利申请
本申请是申请号为08／630，958(1996年4月5日提交)和60／009，876(1995年12月29日提交)两份申请的继续再申请。本发明所属技术领域
本发明涉及利用陶瓷填料床的工艺，在该工艺中，陶瓷填料床用于给流体加热和(或)使流体发生反应，或者充当催化剂的载体。更具体地说，本发明涉及将改进的陶瓷填料用于填料床的工艺。本发明的背景技术
蓄热式加热床被用于吸收并储存灼热的第一流体释放的热量，然后在第二冷流体中发生化学反应(诸如燃烧、氧化、还原或其它化学过程)之前将该热量传送给该冷流体，无论该反应过程是否有催化剂存在。
原先曾经利用砾石作为床的填料。近几十年来，已采用陶瓷的马鞍形填料和填充圈作填料。由于马鞍形填料和填充圈是随机地装填在热交换器的壳体中，它们可能在某个方向上局部地堆积在一起，以致阻断流动。通过充填床的流动是不均匀的，而且流体通过包含马鞍形填料、砾石或环的热交换器引起较高的压力降，通常在10英寸水柱左右。此外，滞留在局部阻断区的流体可能污染流过的第二流体或者被排放到环境中。
最近，在美国专利5，352，115中揭示了在净化燃气的蓄热式氧化系统中使用陶瓷材料整体柱作为热交换柱。这种整体柱的压力降较低，并且减少了在随机装填马鞍形填料或环时经历的污染。
带催化剂层的整体柱还用于合成和将气流转变成其他产物的催化工艺，或用于处理来自内燃机的废气或工业废气。这种陶瓷整体柱上涂覆着催化物质，如稀土金属。但是，这种整体柱的制造成本高。此外，整体柱是刚性的而且是易碎的。在经受反复的加热和冷却之后，该整体柱上的应力裂纹将得以发展，致使整体柱破裂，甚至破碎成小块。于是整体柱不能再继续使用，需要更换新整体柱。在整体柱上涂有稀有金属或稀土金属或涂有包含铂、钯、或铑等的金属化合物时，这种更换的成本可能非常高。此外，整体柱的通道是不透气的，从而导致没有通道内流动气体的横向分散。本发明概述
本发明提供了一种结构与整体柱类似的柱，而它的制造成本只是整体柱成本的一小部分。这种柱由多块陶瓷板组成，而不需要制造均匀的整体柱。陶瓷板可以是经过烧制的，也可以处于原始的未烧制状态。在这些板上有在肋间形成的槽。当这些板被垛起并且板上的肋和槽平行于对置板上的肋和槽时，形成一个具有多个贯穿通道的单元。
板上的肋可以与对置表面衔接。如果对置表面是平的并且这些肋具有相同的高度，那么对置表面与肋的端面接触，形成通道。这些通道可以是不透气的，也可以允许流体横向转移，这取决于在对置表面之间的衔接是否连续。通道的体积和横截面积将由槽的体积和横截面积来确定。这些板有一平的表面，而另一个面有槽。这些板可以是平的，并且它们的形状可以是规则的或不规则的多边形(例如正方形、矩形、三角形、五边形、六边形)或圆形。这些板可以有规则的不对称的横截面或重复的多边形横截面。在板垛中，这些板的尺寸可以是相同的，也可以是按尺寸递增的和(或)按尺寸递减的。这些板可以弯曲成封闭的圆筒并且每块板的外径将比前一块板的外径大，两者的差是前一块板的厚度。所有的槽最好彼此平行，以致这些板可以整齐地垛成柱。这些槽可以平行于一组对置的侧壁，或者与一组对置的端壁形成某个角度(如30°至60°)。
板的尺寸和由板组成的单元尺寸取决于单元的应用目的。如果这些单元准备在汽车的催化反应器中使用，那么这些单元将首尾相接并排地垛成柱。通常，这些单元是由正方形的板形成的矩形单元。通常，这些板的高度可以从0．5英寸至12英寸，宽度可以从1英寸至4英寸。这些板的厚度可以从0．01英寸至1．0英寸，通常是在0．04英寸至0．1英寸之间。单元的高度可以从0．5英寸至50英寸，通常是在1英寸至12英寸之间。
如果这些单元准备在塔中随机充填时使用，那么这些单元的形状最好是多边形，并且通常具有从0．2英寸至5英寸的直径，通常是0．5英寸至3英寸。槽的横截面可以是曲线形、三角形、或矩形。肋的顶端可以是尖的、平的、或者是带圆弧的。为了形成密闭通道而需要粘接较大的接触面积时，最好选用平顶。槽最好尽可能地小并且尽可能地密集。槽的深度和宽度通常介于0．01英寸至1．0英寸之间，最好介于0．04英寸至0．5英寸之间。
单元的另一种组态是将一个或多个肋配置在对置表面的一个槽内，而不是将肋端固定在对置肋的端面上或平坦表面上。肋端伸向槽的底表面，把槽分成两个或多个微型通道。这提供了一种简单而可靠的降低通道尺寸的方法，而不需要通过浇铸或挤压出有非常小的槽板。
本发明的单元包含的陶瓷材料数量与尺寸相同的整体柱包含的陶瓷材料数量大体相同。但是，制造成本却大大降低了。带肋的板可以用压制、浇铸、或挤出方法生产。这些板被切成需要的形状，然后以生料状态或煅烧后的状态堆砌成单元形状。由未煅烧的生料板堆砌的单元需借助煅烧来完成该单元的制造。
当煅烧板垛时，肋与对置肋或壁面接触的部分被熔融成一体。但是，许多不与肋熔接的点起到了消除应力的作用，以适应板的热胀冷缩和防止肋或板破裂，这可能在通道之间形成裂缝。但是，由于反应气体在同一方向上流动，所以没有效率损失。事实上，由于允许气体在通道之间流动，似乎提高了传质效率。在通道之间的开口处锋利的棱边能够干扰边界层，因此，增强了传质作用。借助在板壁上开孔可以进一步增强传质作用和消除应力。通道之间横向的流体渗透和开孔两者都对减少柱中的压力降作出了贡献。陶瓷柱的重复交变应力可能导致裂纹从入口处向柱体延伸。通过适当地缩短肋的长度增加通道入口处的通道宽度，可以减少这种破裂源并且进一步减少压力降。在通道之间的气体分散或许还改善起连接作用的流动。
通过首先烧制陶瓷板来制造这些单元也是可以的。将烧制的陶瓷板垛成一个单元，然后用粘接剂粘或用捆扎物捆使预先烧制的单元稳定。捆扎用的带子或捆扎物可以是金属的，也可以是短效材料，诸如聚乙烯带或偏氯纶带之类的有机塑料膜。这些短效的有机材料在热交换器或单元柱初次加热时被蒸发掉。但是，有机粘接剂(如环氧)和(或)有机膜在蒸发时将氧化碳污染物散发到大气中。最好使用诸如硅酸盐水玻璃之类的耐火的无机粘接剂来粘接该塑制品。将单元垛成有序的柱可能是有利的，其方法是将多个单元装配成多单元结构，具体地说是将单元并排地首尾相接地排列成垛并用粘接剂或诸如线、线网、金属箍圈或金属带之类的机械捆绑器材将这些单元粘接或捆绑成一体。
陶瓷板和单元通常由耐火粘土制成，这类耐火粘土通常包含SiO2、Al2O3、MgO、CaO、K2O2等成分。陶瓷单元对于通过蓄热式热交换器的气体是惰性的并且在反应期间达到的最高温度下仍然保持固体状态。
为了与具有相同表面积的整体柱进行比较，我们进行了试验，其中用于比较的柱是依据本发明由肋板堆砌的单元组成的，并且它们的通道排成一线。出乎意料的是，在采用本发明的单元垛时产出率增加了20％。我们曾经预计产出率将会下降，因为浇铸单元形成的不规则的通道表面将增加流动阻力并降低产出率。或许是由于通道的粗糙表面使毗邻表面的边界层紊乱或干扰该边界层，从而增强了在该边界层中流动的气体之间的混合和反应。
虽然采用装配后再将生料板烧制成单元的方法生产的单元可以消除不衔接点的应力，但是业已发现预先烧制的板组成的单元也一样并且应力裂纹更少。此外，首先烧制陶瓷板然后再将它们装配起来的方式要便宜得多。烧制的刚性板也比软的生料板更容易处理。烧制板上定形的刚性肋还可以压到一起，而且不会引起肋或板变形。生料板中可模塑的软肋在处理或放置时在力的作用下可能发生弯曲和伸缩。
随着结合附图参照下面的详细说明更深入地理解本发明，本发明的这些特征和许多其它特征以及随之而来的优点将变得明朗起来。
附图的简要说明
图1是依据本发明的肋板的第一实施方案的透视图。
图2是由许多图1所示肋板经加热硬化形成的肋板垛组成的单元的透视图。
图3是依据本发明的肋板的另一个实施方案的透视图。
图4是由许多图3所示肋板经加热硬化形成的肋板垛组成的单元的透视图。
图5是肋板的第三实施方案的透视图。
图6是图5所示肋板以单元形式经加热硬化形成的肋板垛的透视图。
图7是肋板的第四实施方案的透视图。
图8是经加热硬化的肋板垛透视图，其中一块图7所示肋板的肋放在对置板的槽内将该槽分成较小的通道。
图9是用短效捆扎物捆绑的一垛经加热硬化的板的主视图。
图10是一垛烧制板的主视图。
图11是靠金属带结合的单元组合件的透视图。
图12是进一步的实施方案的等距图，说明肋板垛的改进方案。
图13是沿着图12中13-13线的剖视图。
图14是压力降曲线对比，其中包括本发明的填充介质、1英寸的马鞍形填料和整体介质。本发明的详细叙述
现在参照图1和图2，其中板10既可以处于生料状态又可以被烧制成硬化状态。硬化的板可以被垛起并用粘接剂将它们粘接起来，或者采用塑料打包带、塑料绳、塑料带或金属箍圈等器材将成垛的板机械地捆绑在一起。无论是处于生料状态的板还是烧制板都可以垛成图2所示的单元12。
板10包含多个从中心部分16的上表面15延伸出来的平行肋14和多个从中心部分16的下表面17延伸出来的平行肋18。槽21和23在毗邻的肋14和14’以及18和18’之间形成。端肋14”和18”的对置端面26和28衔接起来形成端壁22和24。在两端肋之间相邻的对置肋14和18的端面26和28衔接起来形成通道30，通道的体积是槽21和23的体积之和。通道21和23可以是密闭的。气体最好可以通过端面26和28的相交界面向毗邻通道泄漏。正象前面讨论过的那样，可以改变板10的堆砌方式，使肋14和18的对置端26和28插入对置槽21和23，从而将每个槽分成两个通道，而不是使肋14和18的对置端26和28邻接。
现在参照图3和图4，在本发明的第二实施方案中，板110包含从其支撑部分126的上表面122延伸出来的肋114和槽121。板110是这样堆砌的，肋114的端面124与对置板110’的背面128衔接起来，以形成单元140。背面128将肋间的槽121封闭起来形成通道132。端肋130彼此衔接在一起，形成封闭的端壁134。
也可以改变板的堆砌方式，使一些板的肋彼此相对并衔接起来形成更大的通道(未示出)，或者使一些板的肋插到槽中并与槽底衔接形成较小的通道。
现在参照图5和图6，这两张图说明板310和单元312的第三实施方案。肋314和316以及槽318和320平行于对角线中心肋322。在单元312中，肋314和316的端面324和326衔接形成通道328和330。肋也可以与槽交错形成图7所示的较小的通道。
图7所示的板400包含多个从中心部分406的上表面404延伸出来的平行肋402以及多个从中心部分406的下表面410延伸出来的平行肋408。为了形成平坦的侧壁430，对置板424与板400相比，在中心部分428每个面上都少一个肋418’和420’。中心部分428每个面上的第一肋421和422距侧边436的距离为槽432宽度的一半。在板400上肋402和408比槽412和414窄，在板424上也是肋418和420比槽437和438窄，肋的厚度最好不超过毗邻肋(402、408或418、420)之间距离的三分之一。
如8图所示，单元460的装配方法如下：将肋402和408放进对置板424的槽437和438，使肋402和408的端面442和444坐在对置槽437和438的底面446和448上。肋402和408将每个槽437和438分成两个通道450和452。端肋454和456将板424的两个开放端封闭，形成末端小通道462。由未硬化的板装配成的组合件经过烧制形成单元460。板400和424可以预先烧制好，然后再装配成垛460，并借助粘接剂或上述的机械捆绑器材结合成一个单元。
板400和424不需要从每个表面都延伸出肋。板的背面可以是平的。该背面与肋的端面衔接或者与另一块板的背面衔接。槽也可以容纳不止一个肋，例如1至4个肋。单元包含的板可以全是交错的，以形成较小的通道，或者在单元的一些区段中肋与槽是交错的而在另一些区段中肋与对置肋的肋端衔接。还可以有一些板包含一些插入对置槽的长肋和一些与对置肋衔接的短肋。
单元中的板彼此衔接形成脆性的陶瓷体。虽然在肋既不与对置肋端衔接又不与中心支撑内表面衔接的地方有一些运动自由度，但是该单元在蓄热式热处理期间反复地承受加热和冷却时仍然可能破裂、破碎和剥蚀。图9和图10所示的单元500是由错开的板502组成的，这些板之间不是靠烧制或粘接剂衔接起来的。
板502有多个从中心支撑506向下延伸出来的平行肋504，并且中心支撑始于端肋507也止于端肋507。肋508从中心支撑506向上延伸。端肋511从中心支撑的边缘513凹进大约一个端肋507的宽度。当板502和503被垛在一起时，端肋507被锁定在凹进的空间中，它阻止未衔接在一起的板滑动。端肋507与中心支撑506结合形成端壁512。
将每块板一一放入柱中将是费时的。此外，尽管板和板垛被填充在RTO或催化塔或热交换器的壳体中，但是在单独处理板或板垛时破碎仍然时有发生。如图10所示，可以用结实的塑料捆扎物518沿着端壁512、上表面514和下表面516将板垛捆绑到一起，最好使用热缩捆扎物，如Saran(一种乙酸乙烯酯和偏二氯乙烯的共聚物)。然后，将单元520作为一个稳定的整体进行处理放入塔中或者放在类似的垛单元的顶上和(或)与类似的垛单元邻接。当灼热的气体首次进入塔时，捆扎物将分解成气相产物并且伴随着灼热气体从塔中排出。
为了进一步提高塔的装填速度，可以将多个单元520用金属箍圈522捆绑在一起，形成图11所示的组合件524。
单元和模块可以装配成不同尺寸和形状的组合件。该组合件的形态最好是矩形柱或正方形柱。模块可以排列整齐使并排的模块有彼此平行的通道、首尾相接的模块通道有相同的准直轴线。8个6英寸的立方体模块将形成一个1英尺见方的立方体组合件。18个4英寸的立方体模块也将形成一个1英尺见方的立方体组合件。
但是，如上所述，使用有机膜或有机粘接剂将污染环境。有机膜残留的燃烧产物可能留在床中。如图12和图13所示，板540借助硅酸钠或硅酸钾的水溶液(水玻璃)的液膜粘接在一起。水分在室温风干期间从液膜中蒸发，在肋(508和504)的端面534和槽538的底面536之间的接触点上形成硅酸钠和硅酸钾的粘合层532。
未粘合的对置表面允许流动气体在毗邻通道之间横向转移。这有利于提高气体和(或)液体的混合效率、有利于提高单位体积填料的传热和传质效率，以及有利于减少压力降。在板上形成小孔546以增加毗邻通道之间的交流，可以进一步消除应力。扩大通道入口542和削掉肋544的一个短边还将进一步减少压力降。
按照图7的填充模块的制备方法是将涂了水玻璃的烧制陶瓷板堆砌成垛，然后风干形成模块。肋有圆弧形的顶端，肋的高度大约是7．0mm，肋间的间隔大约是7．24mm。
该模块具有下述的尺寸和物理性质：
外形尺寸
层厚 1．5mm
模块的外形尺寸 12”×12”×4”
比表面积 210Ft2／ft3
重量 72Lbs／ft3
空隙因数 60％
物理性质
比重 2．25-2．35
水吸收(ASTMC373) ＜0．5％
耐酸强度，重量损失(ASTMC279) ≤4％
最高的工作温度 2，350°F
热容 0．22BTU／lb°F
低温压碎强度 15，000lbs／ft2
本发明的填充模块的性能与陶瓷整体介质的性能以及1英寸和1／2英寸的马鞍形填料的性能进行过比较。图14所示的数据是利用70°F空气流得到的三种填充介质的压力降对比数据。
对于马鞍形填料在200fpm流速下RTO热回收效率达到95％时的介质深度几乎是本发明介质的
Figure 9619942500152
(8／3)倍，对于整体柱，该介质深度为本发明的多层介质(MLM)的 (5／3)倍。
本发明的MLM介质是用于蓄热式热氧化(RTO)系统的最有效和成本最低的热量回收介质。运行数据证实MLM是数十年来首次超越1英寸的马鞍形填料和整体柱的重大改进。MLM提供了极高的热效率。新的MLM填料在热交换、能效率、和压力降方面的性能超过所有的其它陶瓷介质。它降低了基本投资和运行成本。MLM已经完成了现场试验和实验室试验，并且结果是引人注目的。MLM升温和冷却都比较迅速；与马鞍形填料相比，MLM的薄层形状使其材料集中在表面下1mm范围内。因为通道内部是连通的(与整体柱中彼此隔绝的通道恰恰相反)，所以气体可以在各个方向上流动。这将增强传热以及减少阻塞的倾向。MLM填料是工程技术领域中的一项突破。MLM降低了基本投资和运行成本，而且还能迅速地偿付它本身的费用。
MLM填充材料被认为是数十年来填料设计中最大的进步之一，它为设计调整提供了灵活性。MLM可以在RTO中使用，而且在涉及横向流和高温的传质应用中也是有用的，例如在硫酸厂中它可以用于吸收和干燥；在石油化学厂中可以用于提取、矿物回收、沥滤、溶解和吸收。
应当理解，在这里仅仅介绍了本发明的较佳实施方案，在本发明的权利要求书规定的精神和范围内，允许有许多替代方案、改进方案和变型。

Claims (20)

1．一种用于形成陶瓷填料单元的陶瓷板，其特征在于至少所述板的第一表面包含多个平行肋，在平行肋之间形成平行的槽，从而在所述板与第二板的第一表面邻接时，所述表面与所述槽衔接形成通道。
2．根据权利要求1所述的陶瓷板，其中所述板是平的。
3．根据权利要求1所述的陶瓷板，其中，所述板的另一个表面也包含平行肋和槽。
4．根据权利要求1所述的陶瓷板，其中，所述毗邻肋之间的间隔大于肋的宽度。
5．根据权利要求1所述的陶瓷板，其中所述板处于原始状态。
6．根据权利要求1所述的陶瓷板，其中所述板处于烧结状态。
7．根据权利要求6所述的陶瓷板，其中所述诸表面都包含催化剂层。
8．根据权利要求1所述的陶瓷板，其宽度和深度从0．5英寸至12英寸；其厚度从0．01英寸至1．0英寸。
9．根据权利要求1所述的陶瓷板，其中肋间的板上有通孔。
10．一种陶瓷填料单元，其特征在于包括：
一垛陶瓷板；
一个第一板，该板的第一表面上有多个平行肋，并在平行肋之间形成多个平行的肋间槽；
一个第二板，该板的第一表面与第一板的第一表面紧密接触，以形成平行通道；以及
衔接装置，该装置用于将所述的第一表面结合起来。
11．根据权利要求10所述的陶瓷填料，其中所述衔接装置包括无机粘接剂。
12．根据权利要求10所述的陶瓷填料单元，其中所述肋间的间隔比肋的宽度宽，并且对置表面上的肋是错开的。
13．根据权利要求10所述的陶瓷填料单元，其中所述第二板的第一表面上的肋的间隔大于第一板上的肋的间隔，并且至少有一些所述肋错开且位于对置槽的底表面上。
14．根据权利要求10所述的陶瓷填料单元，其中所述通道具有扩大的入口。
15．一种陶瓷填料组合件，它包括多个由权利要求10定义的填料单元以及紧固这些单元的装置，所述填料单元对准放入一个组件的通道中。
16．根据权利要求15所述的组合件，其中所述系紧装置包括金属带。
17．一种制造陶瓷填料单元的方法，该方法的特征在于包括下述步骤：
在陶瓷板的第一表面上形成多个平行肋和肋间的平行槽；
使第一板的第一表面与第二板的第一表面衔接，以封闭所述槽而形成通道；以及
将第一表面粘接起来。
18．根据权利要求17所述的方法，其中所述陶瓷单元处于烧结状态并且借助无机粘接剂将所有的板粘接起来。
19．一种由板垛组成的陶瓷填料单元，其特征在于板的表面有肋和槽并且包括将该板与毗邻的对置板锁定的装置，以阻止板在垂直于通道的方向上移动，所述装置与板的端肋协作完成板的锁定。
20．根据权利要求19所述的陶瓷填料单元，其中，在第一板上的所述端肋配置在板的两侧，而对置板的端肋是凹进的，凹进深度与第一板上的所述肋厚度相当，借此在第一板装配到对置板上时，第一板的端肋卡住对置板的凹进端肋，从而阻止垂直于通道的移动。
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