CN1444542A - 实现在高温气体介质中反应的新催化设备 - Google Patents
实现在高温气体介质中反应的新催化设备 Download PDFInfo
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Abstract
本发明涉及了一种催化设备,用于实现在高温介质中的反应,例如,HCN的合成或氨的氧化,设备包括:至少一个织构材料(1),可有效地用作上述反应的催化剂,一个支座(2),包括至少一个陶瓷部分(3),其结构可通过气体,上述支座(2)的上述部分(3)具有一个波纹面(6),使得波纹产生的表面积相对于平表面的增加(β)至少等于对锯齿波纹计算的增加(α),在约1.1到约3之间,上述织构材料(1)的位置使得它靠在上述支座(2)的上述部分(3)的波纹面(6)上,并且仿照着它的形状。
Description
本发明涉及了在高温气体介质中的催化反应,例如氨的氧化和HCN的合成。本发明特别主题是一个可以用于这类反应的改进催化设备和一个包括它的反应器。
氨的氧化广泛用于硝酸生产。已知为Ostwald方法的方法包括通过预热氨/空气混合物的阶段,混合物通常包括5-15%,特别是10-12%体积的空气,以高的线性速度(在标准温度和压力条件下度量)通过在反应器横截面上延伸的催化设备。
在单个操作中从氨和气态烃合成氢氰酸(HCN)是一个多年已知的操作(美国专利1,934,838),在存在催化剂下,与氧或含氧气体(如空气)的同时燃烧反应提供了在合成中吸热反应所需的热。这已知为Andrussow方法。
这两类反应采用了铂族催化剂,一般为平的编织网。这些催化剂的表观工作截面受到反应器尺寸的限制。
为了增加这些反应的生产率,可以增加催化网的数目。但是,超过一定的厚度,由此建立的压降阻止了反应物流的增加,并且取消了更好转化产量的效果。此外,厚度的增加会引起副作用。因此,当前技术中提高生产的困难是由于:
-压降;
-催化剂活性部位的数目(接触表面积);
-催化剂与反应物的接触时间。
为了增加催化剂有效表面积,美国专利5,160,722和5,356,603提出了采用具有横向波纹的催化剂网。虽然由此增加了表面积,但这些波纹具有低的波幅。另外,这种设备的形状保持实际上仅在小于800℃下才有可能。超过这个范围,金属的机械特性变得不足,并且由于压降的增加,褶皱或波纹有凹陷的倾向。因此这种设备的寿命非常短,与工业操作不协调。
至于专利申请EP 931,585公布了采用形状为径向波纹盘或锥的催化剂网,使得一个旋转燃烧器在绕其轴线旋转时可以仿照着波纹形状。但是,仍有上述问题。
所以本发明的一个目的是提供一个包括催化剂的催化设备,它具有更大的几何表面积,并且可承受反应条件而基本上不增加压降或副作用。
本发明涉及了一种催化设备,用于实现高温介质中的反应,例如,HCN的合成或氨的氧化,设备包括:
-至少一个织构材料,可有效地用作上述反应的催化剂,
-一个支座,包括至少一个陶瓷部分,其结构可通过气体,上述支座的上述部分具有一个波纹面,使得波纹产生的表面积相对于平表面的增加(β)至少等于对锯齿波纹计算的增加(α),在约1.1到约3之间。
上述织构材料的位置使得它靠在上述支座的上述部分的波纹面上,并且仿照着它的形状。
使织构材料靠在支座部分的波纹面上的装置最好是由陶瓷支座的一个第二部分组成,其结构可以通过气体,上述第二部分具有一个波纹面,它与支座的上述第一部分的上述波纹面基本上为异体同构和互补,以及上述第二部分的位置使得上述第一和第二部分的上述波纹面面对面,并且使得织构材料插入上述波纹面之间和仿照着它们的形状。因此,沿着由此形成的整个催化设备,压降有利地基本均匀。
可以采用对熟悉该技术的人员已知的其他常规装置来把织构材料靠在支座第一部分的波纹面上。
在本发明的意义中,名称“织构材料”理解为带或丝的任何集合物,它们为可以通过气体的线状和/或螺旋形状的部件。例如,这种集合物为网、编织织物、编结织物或毡类,并且可以用各种技术得到、如编织、编结、缝纫、刺绣之类,最好是一个网。
在本发明的意义中,名称“两个基本上为异体同构和互补形状的波纹面”理解为两个具有相似尺寸和形状的波纹面的任何组合,也就是说,具有基本上相同的表面积增加β,当这两个面面对时,它们被构成使得波纹为互补。
从以下的详细描述和依靠参照以下的说明图例,本发明的其他主题和优点对熟悉该技术的人员将会变得很明显。
图1代表了本发明催化设备的一个简略的具体例子。
图2代表了可用于计算由锯齿波纹产生的表面积增加(α)。
本发明的支座(2)由陶瓷做成,它的结构可以通过气体。这些陶瓷之例为(但不限于)泡沫陶瓷和复合陶瓷。支座(2)可以为一个蜂窝结构。在本发明的意义中,名称“陶瓷”最好理解为任何耐熔材料,它在尤其包括蒸汽的反应介质中能够承受催化铂网产生的温度。在按照Andrussow方法的HCN合成中应用的情形,这个温度可以达到1200℃。因此适用的材料均以刚玉为基础,并且可以包括不同比例的硅(重量10到60%)和镁、锆、钛和铈的氧化物(对这些成分的每一个为重量1到20%)。这些材料可以包括(但不限于)以下化合物的一个和几个:二氧化硅(石英,SiO2)、碳化硅SiC、氮化硅Si3N4、硼化硅、氮化硼硅、氧化铝(刚玉,Al2O3)、硅铝酸盐(3Al2O3-2SiO2)、硅铝硼酸盐、碳纤维、氧化锆(ZrO2)、氧化钇(Y2O3)、氧化钙(CaO)、氧化镁(MgO)和堇青石(MgO-Al2O3-SiO2)。
最好采用Stettner生产的陶瓷StettaG29,其特征如下:
孔隙率% | 相对密度kg/dm3 | 弯曲强度N/mm2 | 线膨胀系数1×10-6/K在20-200℃ | 线膨胀系数1×10-6/K在20-600℃ | 热导率W/(mK) | 抗热冲击℃ | 最大工作温度℃ | 体积电阻在800℃ |
>3 | 2 | 45 | 1.5-3 | 2-4 | 1.3-1.7 | 380 | 1000 | 105 |
在使用它们之前,按照已知的模制、挤压、烧结等技术成形这些用于形成支座(2)的材料。接着在高温(>1300℃)下煅烧它们,从而得到与它们以后工作条件相容的机械性质。这些组合的操作必须给它们一个可通过气体的结构,例如,具有沿三个方向连通的小格子形状(泡沫)或者具有圆形或多边形(正方形、矩形、六角形等)截面的蜂窝。
有效地用作催化剂的织构材料(1)特别是为一种铂族的催化金属,可以从铂、铑、铱、钯、锇、钌,或者从两个或更多的这些金属的混合物或合金来制备。最好采用铂或铂/铑合金。或者是,这种催化剂可以是上述一个铂族催化剂和至少一个其他材料的混合物,其他材料包括(但不限于)铈、钴、锰、镁和陶瓷。
支座面(6)和(7)的波纹可以为任何类型,特别是为锯齿形波纹。
锯齿形波纹由每个波纹的高度“h”和两个波纹之间的距离“d”来确定。因此可以按以下方式从这两个参数(图2)来计算这类波纹产生的表面积增加α:
本发明的任何类型波纹产生的表面积增加(β)将至少等于(α),并且在范围1.1到3之内选择。这是因为α=1.1相应于表面积增加10%。低于这个值,这种波纹的优点不太明显。高于β=3,采用这种设备变得很困难。本发明的锯齿形波纹最好为具有d=2h的等腰三角形外形,它产生约为1.40的比值α,因此增加表面积约40%。
本发明还涉及了一个反应器,用于在气体介质中的高温放热反应,具有一个大致为圆形的横截面,其特征在于:它包括了沿其横截面延伸的本发明催化设备。
它还涉及了在高温气体介质中的反应方法,如氨的氧化或HCN的合成,其特征在于:它利用了本发明的催化设备或反应器。
在本发明的一个具体实施例中,本发明的方法是HCN的合成,包括了在800和1400℃之间的温度下把包括烃(最好是甲烷、氨和氧)的气体混合物通过本发明催化设备的一个阶段,从而在反应之后得到一个至少含5%体积HCN的气体流。
用于本发明HCN合成方法的烃可以是一个取代或未取代以及脂族、环族或芳香族的烃,或者其混合物。这些烃的例子包括(但不限于)甲烷、乙烯、乙烷、丙烯、丙烷、丁烷、甲醇和甲苯。烃最好是甲烷。
本发明还涉及了制备本发明催化设备的方法,其特征在于:把织构材料(1)铺平靠在支座(2)部分(3)的波纹面(6)上,使得它仿照其形状,以及利用一个固定装置把它保持在那里。
这个固定装置最好是机械的,由支座(2)的第二部分(4)组成,它的波纹面(7)覆盖了上述材料(1)的面,这个面背对着靠在上述支座(2)部分(3)波纹面(6)上的面。
更有利的是,由此形成的组合产生了在反应器截面中基本上均匀的低压降。
本发明设备的一个简略的具体例子(图1)包括:
-一个波纹网(1)的组合,
-一个分成两个部分(3)和(4)的波纹陶瓷支座(2),每个部分具有一个波纹面(6)和(7)。
网(1)位于支座(2)的部分(3)和(4)的两个面(6)和(7)之间。
支座(2)的部分(3)和(4)由陶瓷做成,具有为圆形或多边形(正方形、矩形、六角形等)截面的蜂窝结构。
制备本发明催化设备的例子:
可以把具有三角形截面的棱柱装配和胶接在一起,在煅烧之前(在模制时)或在煅烧之后对本发明的支座(2)给出一个波纹形状。
接着把构成催化剂的一组铂网(1)插入波纹支座(2)的两个层(3)和(4)之间。这个定位操作进行如下:在支座(2)的波纹部分(3)上,把将铺到支座部分(3)波纹上的一组椭圆形网(1)铺平,支座已经事先定位在构成圆截面反应器基础的空心砖(11)上。椭圆网的宽度相应于反应器的内径。长度等于宽度乘以先前确定的系数β。波纹材料的上层(4)可以机械地固定网(1),同时对整个露出表面上的组合给出均匀的压降。接着把一个防热层(10)放在由此形成的催化设备上。可以把反应和所有活性能限制到网(1)表面的最近点上。空心砖(11)本身位于反应器的锅炉管道(12)上,由耐热水泥(13)组成。性能
本发明催化设备的应用使得对相同反应器有可能增加催化剂和反应物之间的接触表面积。对于相同的反应物总流量,这造成了改进的生产率以及最小和基本不变的压降,可能使生产使用周期更长,并且将更加如此,因为这种设备可承受反应条件,特别是不会引起机械变形。
下表可以把一个先前技术的代表性系统与本发明的催化设备作比较。
先前技术平系统 | 本发明波纹系统 | |
系数α | 1.0 | 1.4 |
生产率:每吨空气和每公斤催化剂的HCN(公斤) | 2.0 | 2.16 |
压降的增加:初始压降的每月增加(%) | 29 | 5 |
试验时间:生产小时 | 993 | 3138 |
Claims (14)
1.一种催化设备,用于实现在高温介质中的反应,例如,HCN的合成或氨的氧化,设备包括:
-至少一个织构材料(1),可有效地用作上述反应的催化剂,
-一个支座(2),包括至少一个陶瓷部分(3),其结构可通过气体,上述支座(2)的上述部分(3)具有一个波纹面(6),使得波纹产生的表面积相对于平表面的增加(β)至少等于对锯齿波纹计算的增加(α),在约1.1到约3之间。
上述织构材料(1)的位置使得它靠在上述支座(2)的上述部分(3)的波纹面(6)上,并且仿照着它的形状。
2.按照权利要求1的催化设备,特征在于:使材料(1)靠在支座(2)部分(3)的波纹面(6)上的装置由陶瓷支座(2)的一个第二部分(4)组成,其结构可以通过气体,上述部分(4)具有一个波纹面(7),它与上述部分(3)的上述波纹面(6)基本上为异体同构和互补,以及上述部分(4)的位置使得上述波纹面(6)和(7)面对面,并且使得材料(1)插入上述面(6)和(7)之间和仿照着它们的形状,因此沿着由此形成的整个催化设备,压降有利地基本均匀。
3.按照以上权利要求中任一条的催化设备,特征在于:支座(2)具有一个蜂窝结构。
4.按照以上权利要求中任一条的催化设备,特征在于:波纹为锯齿形,使得表面积的增加β=表面积的增加α。
5.按照权利要求4的催化设备,特征在于:表面积的增加β约为1.4。
6.按照以上权利要求中任一条的催化设备,特征在于:材料(1)为一个网。
7.在气体介质中高温放热反应的反应器,具有大致为圆形的横截面,特征在于:它包括一个如在权利要求1到6中规定的催化设备,设备沿着其横截面延伸。
8.按照权利要求7的反应器,特征在于:放热反应是HCN的合成。
9.按照权利要求8的反应器,特征在于:设备放在构成反应器基础的空心砖(11)上,并且用一个防热层覆盖。
10.在高温气体介质中的反应方法,特征在于:采用如权利要求1到6规定的催化设备或权利要求7到9规定的反应器。
11.按照权利要求10的方法,特征在于:它是HCN的合成。
12.按照权利要求11的方法,特征在于:它包括了在800和1400℃之间的温度下把包括烃(最好是甲烷、氨和氧)的气体混合物通过按照权利要求1到6的催化设备的一个阶段,从而在反应之后得到一个至少含5%体积HCN的气体流。
13.制备按照权利要求1到6的催化设备的方法,特征在于:把织构材料(1)铺平靠在波纹支座(2)部分(3)的表面(6)上,使得它仿照其形状,以及利用一个固定装置把它保持在那里。
14.按照权利要求13的方法,特征在于:固定装置是机械的,由支座(2)的部分(4)组成,它的表面(7)覆盖了上述材料(1)的表面,这个表面背对着靠在上述支座(2)部分(3)表面(6)上的表面。
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CN103864114A (zh) * | 2012-12-18 | 2014-06-18 | 英威达科技公司 | 采用催化剂床层生产氰化氢的方法 |
CN113603115A (zh) * | 2012-12-18 | 2021-11-05 | 英威达纺织(英国)有限公司 | 采用催化剂床层生产氰化氢的方法 |
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UA74202C2 (uk) | 2005-11-15 |
PL365139A1 (en) | 2004-12-27 |
JP5000065B2 (ja) | 2012-08-15 |
HUP0301700A2 (en) | 2003-08-28 |
US20030175195A1 (en) | 2003-09-18 |
JP2004504939A (ja) | 2004-02-19 |
SK285674B6 (sk) | 2007-06-07 |
MXPA03000858A (es) | 2004-12-13 |
KR100680848B1 (ko) | 2007-02-08 |
HU227856B1 (en) | 2012-05-02 |
FR2812221B1 (fr) | 2003-04-04 |
US7101525B2 (en) | 2006-09-05 |
DE60122344D1 (de) | 2006-09-28 |
RU2257949C2 (ru) | 2005-08-10 |
CN1266042C (zh) | 2006-07-26 |
SK952003A3 (en) | 2004-06-08 |
CA2423030A1 (en) | 2002-02-07 |
EP1307401A1 (en) | 2003-05-07 |
WO2002010067A1 (en) | 2002-02-07 |
CA2423030C (en) | 2009-01-13 |
FR2812221A1 (fr) | 2002-02-01 |
BR0112822B1 (pt) | 2010-11-03 |
PL205555B1 (pl) | 2010-05-31 |
ATE336463T1 (de) | 2006-09-15 |
EP1307401B1 (en) | 2006-08-16 |
BR0112822A (pt) | 2003-07-01 |
AU2001286159A1 (en) | 2002-02-13 |
CZ304571B6 (cs) | 2014-07-16 |
KR20030081298A (ko) | 2003-10-17 |
DE60122344T2 (de) | 2007-08-09 |
CZ2003174A3 (cs) | 2003-10-15 |
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