CN111372675A - 具有集成的热交换器的化学反应器 - Google Patents

具有集成的热交换器的化学反应器 Download PDF

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CN111372675A
CN111372675A CN201880075546.XA CN201880075546A CN111372675A CN 111372675 A CN111372675 A CN 111372675A CN 201880075546 A CN201880075546 A CN 201880075546A CN 111372675 A CN111372675 A CN 111372675A
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catalyst
chemical reactor
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heat exchanger
barium calcium
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CN111372675B (zh
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J·D·比奇
J·D·金特纳
A·W·韦尔奇
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Spark Energy
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Abstract

公开了一种将压力容器、热交换器、加热器和催化剂支持器组合入单个装置的化学反应器。本文所述的化学反应器降低了反应器的成本并且降低了其寄生热损失。公开的化学反应器适用于氨(NH3)合成。

Description

具有集成的热交换器的化学反应器
相关申请的交叉引用
本申请根据35U.S.C.§119(e)要求于2017年11月25日提交的美国临时专利申请序列号62/590,570的优先权和权益。美国临时专利申请序列号62/590,570在此通过引用以其全部并入本文。
技术领域
本公开内容涉及将热交换器、加热器和催化剂支持器(catalyst holder)集成入单件设备的化学反应器设计。在一些实施方案中，本文公开的化学反应器适用于氨(NH3)合成。
背景技术
由二氧化碳(CO2)的人为排放驱动的气候变化对持续的经济发展和安全造成的威胁是本领域技术人员熟知的。为了应对这种威胁，发达国家和发展中国家均高度寻求基本上没有CO2排放的能源。虽然已经广泛开发了几种无CO2的能量生成选择(例如风能、太阳能、水电和核电)，但是目前没有包括可实行的无CO2的燃料。
氨(NH3)可以根据以下反应式(1)作为燃料燃烧：
4NH3(g)+3O2→2N2+6H2O(g)+热 (1)
原则上，如果将NH3热重整为氢气和氮气，那么NH3可以被直接用作无CO2的燃料或用作储氢(hydrogen storage)介质。然而，几乎所有当前的NH3生产方法均使用产生CO2的原料和燃料。
生产氨的主要工业过程是在以下反应式(2)中示例的哈伯-博施(Haber-Bosch)方法：
N2(g)+3H2(g)→2NH3(g)(△H＝-92.2kJ/mol) (2)
在2005年，每生产1吨NH3，哈伯-博施氨合成产生平均大约2.1吨CO2；大约三分之二的CO2产生来自烃的蒸汽重整(steam reforming)以生产氢气，而剩余的三分之一来自烃燃料燃烧以给合成工厂提供能量。到2005年，大约75％的哈伯-博施NH3工厂使用天然气作为进料和燃料，而剩余的使用煤或石油。哈伯-博施NH3合成消耗了全球天然气产量的大约3％至5％以及全球能量产量的大约1％至2％。
哈伯-博施反应通常在含有氧化铁或钌催化剂的反应器中在大约300℃和大约550℃之间的温度并且在大约90巴(bar)和大约180巴之间的压力下进行。需要升高的温度以实现合理的反应速率。由于NH3合成的放热性质，升高的温度驱动平衡朝向反应物，但是这被高压抵消。在商业生产中，来自氨合成的废热促进通过蒸汽重整天然气的制氢。
氨合成的最新进展已经产生了可以在大约300℃和大约600℃之间的温度并且在1巴直至压力容器与压缩机设计的实际限度的范围内的压力下操作的反应器。当设计用于较低操作压力时，该新一代反应器可以降低设备成本和气体压缩成本，但是它们还降低在每次通过催化剂床(catalyst bed)期间转化成NH3的N2和H2反应物的分数。这增加了形成给定量的NH3所需的再循环的次数，这可以增加给定量的NH3的热损失，除非使用合适的热交换器高效地再循环反应器热。除非使用具有高气体传导性的催化剂床，否则较高数目的反应物再循环也可以增加循环泵能量需要。
本领域需要如下NH3反应器设计，其(a)集成催化剂床和热交换器以最小化热损失，(b)集成加热器以向反应提供补充热(make-up heat)，和(c)使用高传导性催化剂床设计以降低反应物再循环能量需要。这样的设计将降低资金成本并且能够实现低压NH3反应器所需要的高再循环分数。
发明内容
本发明内容是为了以简化的形式介绍将在以下具体实施方式中进一步描述的一些概念。本发明内容以及前述背景技术并非旨在标识所要求保护的主题的关键方面或必要方面。此外，本发明内容并不旨在用于帮助确定所要求保护的主题的范围。
本公开内容描述了一种化学反应器，比如适用于由N2和H2反应物气体产生NH3的化学反应器。本文所述的化学反应器将压力容器、热交换器、加热器和高传导性催化剂床集成入单个装置以减小系统尺寸、降低系统成本并且减少寄生热损失(parasitic heat loss)。本文所述的化学反应器可以被用于在升高的压力和温度下使用多相催化由气体合成各种化合物，包括但不限于由N2和H2反应物气体合成NH3。
在考虑本文的具体实施方式和附图后，本文描述的化学反应器的这些和其他方面将是清楚的。然而，应当理解，要求保护的主题的范围应当由所公布的权利要求来确定，而不是由给定的主题是否解决了背景技术中所述的任何或所有问题或者包括发明内容中所述的任何特征或方面来确定。
附图说明
参考以下附图描述公开的化学反应器的非限制性和非穷尽性实施方案，包括优选实施方案，其中除非另外指明，否则在各个视图中，相同的附图标记表示相同的部件。
图1A是根据本文描述的各种实施方案的组合式热交换器、加热器和催化剂支持器装置的径向横截面视图。
图1B是图1A中所示的组合式热交换器、加热器和催化剂支持器装置的轴向横截面视图。
图2是根据本文所述的各种实施方案的使用棒状加热器和环形圆筒(cylinder)催化剂支持器的组合式热交换器、加热器和催化剂支持器装置的轴向横截面视图。
图3是根据本文所述的各种实施方案的使用圆柱体加热器和金属单体(monolith)催化剂支持器的组合式热交换器、加热器和催化剂支持器装置的轴向横截面视图。
图4是根据本文所述的各种实施方案的组合式热交换器、加热器和催化剂支持器装置的轴向横截面视图，其中金属单体用作加热器和催化剂支持器两者。
具体实施方式
下面将参考附图更全面地描述实施方案，附图形成了实施方案的一部分，并且以说明的方式示出了具体的示例性实施方案。这些实施方案被充分详细地公开以使得本领域技术人员能够实践所公开的实施方案。然而，实施方案可以以许多不同的形式实现，并且不应当被解释为受限于在此阐述的实施方案。因此，下面的具体实施方式不是限制性的。
本文描述了单一化学反应器装置的各种实施方案，该单一化学反应器装置包括含有逆流螺旋式热交换器、加热器和催化剂支持器的压力容器。该设计适用于NH3合成，也可以应用于其他高温气相多相催化反应。为了描述公开的化学反应器，将参考化学反应器在NH3合成中的应用。然而，公开的化学反应器不应当被解释为仅适用于NH3合成。
参见图1A，示出了根据本文描述的各种实施方案的装置100的径向横截面。圆柱体压力容器110具有附接至其内表面111的螺旋式热交换器120。反应物气体经由压力容器110侧面的端口112(在图1A中也标记为“反应物输入”)进入螺旋式热交换器冷侧(cold side)入口121。当反应物气体向内螺旋通过螺旋式热交换器120至装置100的中心区域101时，反应物气体获得热量，如下面更详细地讨论的，该装置100的中心区域101包含加热器和催化剂支持器(图1A中未显示)。
如下面更详细地讨论的，可以布置在中心区域101中的加热器在装置预热期间向反应物提供热量并且补偿寄生热损失，使得反应物可以保持在期望的温度(通常300-600℃)。如下面更详细地讨论的，可以布置在中心区域101中的催化剂支持器是发生NH3合成的位置。包含在催化剂支持器中的催化剂可以是促进期望的反应的任何合适的催化剂。当期望的反应是氨合成时，催化剂可以包括促进铁(promoted iron)氨合成催化剂、金属修饰的(metal-decorated)钡钙铝氧化物催化剂、金属修饰的钡钙硼氧化物催化剂或金属修饰的钡钙铝硼氧化物催化剂。更具体地，催化剂可以是粒状的(granular)促进铁氨合成催化剂、粒状或丸状的(pellet)金属修饰的钡钙铝氧化物催化剂、粒状或丸状的金属修饰的钡钙硼氧化物催化剂、粒状或丸状的金属修饰的钡钙铝硼氧化物催化剂、分散在氧化铝颗粒上的金属修饰的钡钙铝氧化物催化剂的粉末、分散在氧化铝颗粒上的金属修饰的钡钙硼氧化物催化剂的粉末或分散在氧化铝颗粒上的金属修饰的钡钙铝硼氧化物催化剂的粉末。
在通过布置在中心区域101中的加热器和催化剂支持器后，产物气体进入螺旋式热交换器120的热侧(hot side)入口122。当产物气体朝向螺旋式热交换器120的冷侧出口123(在图1A中也标记为“产物输出”)向外螺旋时，它们的热量被传递至进入的反应物。冷却的产物气体离开装置100并且流动至其他装置(其从产物气体流提取NH3)，而非本文所述的化学反应器的一部分。
参见图1B，示出了图1A的组合式热交换器、加热器和催化剂支持器装置100的轴向横截面视图。在此视图中可见压力容器110的顶部和底部被凸面法兰(convex flange)130密封。反应物气体经由端口112(显示在图1B中的装置100的右侧上)进入反应器100。螺旋式热交换器120的外部的“反应物输入”螺旋部分中的压力平衡端口124允许在螺旋式热交换器120的上方和下方并且在凸面法兰130下轴向定位的隔离空间(insulated space)131被反应物气体加压。将顶部和底部压力平衡端口124均定位在螺旋式热交换器120的反应物入口螺旋的开始处确保它们处于与进入的反应物相同的压力下，防止通过它们的连续流动，并且防止它们提供反应物绕过螺旋式热交换器120、加热器(图1B中未显示)和催化剂支持器(图1B中未显示)的路径。
平衡隔离空间131和螺旋式热交换器120中的压力允许装置100在压力下操作而不会在螺旋式热交换器120的热交换器螺旋中产生机械负载。这是有利的，因为它允许螺旋式热交换器的螺旋壁由较薄的材料区段构建，降低了装置成本和重量并且增加了反应物输入流和产物输出流动之间的热交换率。例如，在10巴的压力下操作的不具有平衡的内部压力和外部压力的螺旋式热交换器可能需要0.9mm厚的钢螺旋以承受压力引起的应力，而具有平衡压力的热交换器可以使用0.1mm的钢螺旋，这是因为它们只需要支撑热交换器重量。压力平衡还因为如下是有利的：允许在隔离空间130中使用高效的可压缩隔离材料，比如矿棉和陶瓷纤维。如果不使用压力平衡端口124，则不可压缩的隔离材料可以被用于将力从催化剂支持器(图1B中未显示)和螺旋式热交换器120传递至压力容器110的壁。由于周围的轮、轮胎侧壁和轮胎胎面提供了机械强度，这可以允许螺旋式热交换器120仍由较薄的材料区段构建，其方式与如何将薄的内管充气至高压类似。
在操作中，冷的反应气体进入装置100并且冷的产物气体离开装置100。在装置100的中心区域101处，仅加热器(图1B中未显示)、催化剂支持器(图1B中未显示)和与它们相邻的区域是热的。这允许压力容器110的外壁保持在环境温度。加热器(图1B中未显示)、催化剂支持器(图1B中未显示)和螺旋式热交换器120上方和下方的区域填充有隔离材料，其允许压力容器110的顶壁和底壁保持在环境温度。将压力容器110的壁保持在环境温度是有利的，这是因为其允许它们由具有较低温度限制的较低成本材料的较薄区段构建。与具有热的外壁的装置相比，降低了装置100的成本和重量。
如上面参考的，图1A和1B中显示的装置100的中心区域101可以包括加热器和催化剂支持器。加热器和催化剂支持器的具体配置可以变化。图2-4示出了可以在图1A和1B所示的装置100中使用的各种加热器和催化剂支持器配置。
参考图2，示出了一个加热器和催化剂支持器配置实施方案的轴向横截面视图。在此实施方案中，催化剂支持器240是具有穿孔的内壁241和穿孔的外壁242的环形圆筒。催化剂支持器240的环形区域243填充有粒状的NH3催化剂。穿孔的壁241、242允许气体径向地流动通过填充环形区域243的催化剂。加热器250是棒状的并且位于环形催化剂支持器240的中心处。
在操作中，反应物气体经由“反应物输入”端口112(显示在图2中的右侧上)进入反应器100。反应物气体朝向反应器100的中心区域101流动通过螺旋式热交换器120的螺旋通道。当反应物朝向装置100的中心区域101流动时，它们从朝向装置100的边缘流动通过螺旋式热交换器120的产物获得热量。在“反应物输入”向内行进通过催化剂支持器240的外侧附近的螺旋式热交换器120的位点处，螺旋式热交换器120终止并且接合穿过环形催化剂支持器240的管组244，以将加热的反应物递送至催化剂支持器240的开口中心(open center)。反应物撞击在位于那里的加热器250上，从而允许它们在需要时被加热。然后反应物从催化剂支持器240的中心区域101(任选地，经由加热器250加热)流动通过发生NH3合成的催化剂支持器240。产物气体(未使用的反应物+NH3反应产物)被收集在正好在环形催化剂支持器240的外部的区域245中(在图2中也标记为“产物输出”)。然后它们进入螺旋式热交换器120的“产物输出”螺旋。当产物气体流动通过“产物输出”螺旋时，它们的热量被传递至流动通过“产物输入”螺旋的进入的反应物。产物气体经由“产物输出”端口113(显示在图2的左侧上)离开装置100。
图3示出了催化剂支持器和加热器配置的另一个实施方案。反应物进入装置100并且朝向装置100的中心区域101流动通过螺旋式热交换器120，这样从产物流获得热量。在装置100的中心区域101处，反应物轴向地通过加热器350，如果需要，加热器350向反应物添加补充热。加热器的非限制性实例包括蜂窝单体、带翅片的螺旋杆加热器或带翅片的蛇形杆加热器，每种均通过电流进行加热。
然后，充分加热的反应物轴向地流入在加热器350的下游轴向地定位的催化剂支持器340。催化剂支持器340是涂覆有NH3合成催化剂的蜂窝状片材金属或箔单体，类似于金属单体自动催化转化器(automotive catalytic converter)。反应物与催化剂相互作用以制备NH3，并且得到的产物气体和未使用的反应物进入螺旋式热交换器120的“产物输出”螺旋。当反应物经由螺旋式热交换器120的“产物输出”螺旋朝向装置100的外缘流动时，它们的热量被传递至向内流动通过螺旋式热交换器120的进入的反应物。
图4示出了催化剂支持器和加热器配置的又一个实施方案。气体以与图3描述的相同方式流动通过装置100。然而，在此实施方案中，加热器和催化剂支持器被组合入单个金属单体440。金属单体440由薄的片材金属或箔制成并且涂覆有NH3合成催化剂。配置金属单体440以使得电流可以穿过它以加热它和所附的催化剂。这是有利的，因为允许单体440替换在图3中描绘的单独的加热器350，减少了设备零件数。还有利的是，催化剂与单体440的直接结合允许催化剂被非常快速地加热，减少了装置开始生产NH3需要的时间。
从上文可以理解，为了说明的目的，本文已经描述了公开的化学反应器的具体实施方案，但是在不偏离公开的化学反应器的范围的情况下可以进行各种修改。因此，除了所附权利要求外，公开的化学反应器不受限制。
尽管已经使用特定于某些结构和材料的语言描述了该技术，但是应当理解，所附权利要求中限定的化学反应器不必限于描述的特定结构和材料。更确切地说，这些具体方面被描述为实施所要求保护的化学反应器的形式。因为化学反应器的许多实施方案可以在不脱离化学反应器的精神和范围的情况下实施，所以化学反应器存在于此后所附的权利要求中。

Claims (14)

1.一种化学反应器，包括：
压力容器；
布置在所述压力容器内的螺旋式热交换器，所述螺旋式热交换器包括：
中心区域；
反应物输入螺旋通道，其配置为将反应物从所述螺旋式热交换器的入口端口传递至所述中心区域；和
反应物输出螺旋通道，其配置为将反应物从所述中心区域传递至所述螺旋式热交换器的出口端口；
加热器，其布置在所述压力容器内并且在所述螺旋式热交换器的所述中心区域中定位；和
催化剂支持器，其布置在所述压力容器内并且在所述螺旋式热交换器的所述中心区域中定位。
2.根据权利要求1所述的化学反应器，其中所述催化剂支持器是环形催化剂支持器，并且所述加热器在所述环形催化剂支持器内定位。
3.根据权利要求2所述的化学反应器，其中所述环形催化剂支持器包括穿孔的外壁和内壁。
4.根据权利要求3所述的化学反应器，其中所述环形催化剂支持器包括延伸通过所述催化剂支持器的管。
5.根据权利要求1所述的化学反应器，其中所述加热器在所述中心区域的一个轴向端处定位，并且所述催化剂支持器在所述中心区域的相对的轴向端处定位。
6.根据权利要求5所述的化学反应器，其中所述反应物输入螺旋通道的出口端靠近所述加热器的上游侧定位，并且所述反应物输出螺旋通道的入口端靠近所述催化剂支持器的下游侧定位。
7.根据权利要求5所述的化学反应器，其中所述催化剂支持器包括涂覆有催化剂的具有蜂窝状结构的片材金属或箔单体。
8.根据权利要求1所述的化学反应器，其中所述加热器和所述催化剂支持器被集成入相同的单体部件。
9.根据权利要求8所述的化学反应器，其中所述单体部件是具有蜂窝状结构的片材金属或箔单体，所述片材金属或箔单体涂覆有催化剂并且配置为通过使电流穿过所述单体而进行加热。
10.根据权利要求1所述的化学反应器，其中所述催化剂支持器包含粒状的催化剂。
11.根据权利要求1所述的化学反应器，其中所述催化剂支持器包括促进氨合成的催化剂。
12.根据权利要求4所述的化学反应器，其中所述催化剂支持器包含催化剂，并且所述催化剂选自由如下组成的组：粒状的促进铁氨合成催化剂、粒状或丸状的金属修饰的钡钙铝氧化物催化剂、粒状或丸状的金属修饰的钡钙硼氧化物催化剂、粒状或丸状的金属修饰的钡钙铝硼氧化物催化剂、分散在氧化铝颗粒上的金属修饰的钡钙铝氧化物催化剂的粉末、分散在氧化铝颗粒上的金属修饰的钡钙硼氧化物催化剂的粉末和分散在氧化铝颗粒上的金属修饰的钡钙铝硼氧化物催化剂的粉末。
13.根据权利要求7所述的化学反应器，其中所述金属单体上的催化剂是金属修饰的钡钙铝氧化物催化剂、金属修饰的钡钙硼氧化物催化剂、金属修饰的钡钙铝硼氧化物催化剂或其组合。
14.根据权利要求9所述的化学反应器，其中所述金属单体上的催化剂是金属修饰的钡钙铝氧化物催化剂、金属修饰的钡钙硼氧化物催化剂、金属修饰的钡钙铝硼氧化物催化剂或其组合。
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