CN1250446C - 含高级烃的烃进料自热转化的方法 - Google Patents

含高级烃的烃进料自热转化的方法 Download PDF

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CN1250446C
CN1250446C CNB991202589A CN99120258A CN1250446C CN 1250446 C CN1250446 C CN 1250446C CN B991202589 A CNB991202589 A CN B991202589A CN 99120258 A CN99120258 A CN 99120258A CN 1250446 C CN1250446 C CN 1250446C
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T·S·克里斯滕森
J－Hb·汉森
P·S·克里斯滕森
I·I·普里姆达尔
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Abstract

一种用于在自热转化器中通过含高级烃的烃进料的催化自热转化制备富氢和/或一氧化碳气的方法，还包括步骤：(a)将烃进料通过含蒸气转化催化剂的第一反应器以除去或减少烃进料中的高级烃含量；(b)将从第一反应器中得到的流出物通入自热反应器中；和(c)从自热转化器中取出富氢和/或一氧化碳的产品气。

Description

含高级烃的烃进料自热转化的方法
本发明涉及含高级烃的烃进料无烟灰自热转化(ATR)。
在自热转化中，烃进料的燃烧是在炉燃烧区段用焰火反应与低于化学计算量的氧进行的，接着部分燃烧后的进料在蒸气转化催化剂的固定尿中蒸气转化。烃的亚化学计量燃烧导致有害的烟灰形成。通过使用专门的燃烧炉设计和通过控制ATR方法的操作条件，烟灰的形成可以被克服。烟灰是在一定范围的操作条件内在自热反应器的火焰中形成的。当蒸气量相对于送入ATR反应器中的其它组分是在临界值以下时，在反应的进料中形成烟灰。一种用于ATR的这种燃烧炉叙述于美国专利5,496,170中。蒸气的限制量可以表示成蒸气与碳的临界比，该比值是蒸气的摩尔进料流速与在烃进料中碳的摩尔流速之比。烃进料可以是以天然气或包括LPG、丁烷、石脑油等烃的形式。碳的摩尔流速以烃的摩尔流速乘烃的含碳量计算。
不会造成烟灰形成的操作条件的实例已由Christensen和Primdahl总结在论文中(《烃加工》1994年3月39-46页)。这些条件表示于表1中。这些试验在中试装置中进行。由于从相对小的中试装置的热损失，绝热ATR出口温度将高于测得的ATR出口温度。这意味着如若大装置(从中热损失是很小的)经受严格相同的操作条件，那么ATR出口温度将接近绝热ATR出口温度。烟灰产物母体是在ATR的燃烧区段形成的。大多数热损失在燃烧区段后出现其后的热损失对燃烧区段中的反应物不会有任何影响。氧与碳比(O2/C)也表示于表1中。此比值的定义类似于蒸气与碳之比，但用氧替代蒸气。ATR反应器的出口温度可以由O2/C之比计算，当从反应器的热损失已知时。
表1
  例号   氧与碳之比   H2O/C   CO2/C  测得ATR出口温度℃  绝热ATR出口温度℃
  A   0.60   1.43   0  950  1013
  B   0.62   0.59   0  1065  1173
  C   0.60   0.86   0  1000  1073
  D   0.67   0.68   0.47  1018  1147
  E   0.70   0.67   0.75  1030  1147
  F   0.73   0.58   0.98  1028  1177
不造成烟灰形成的操作条件(取自Christensen和Primdahl论文，1994年)。
有利地是在低的蒸气与碳比值操作本方法，因为低比值减少了ATR装置的投资费用并降低了操作装置的必须能量消耗。此外，低的蒸气与碳比值使它可能优化生成的合成气组合物，该合成气组合物用于如甲醇或二甲醚合成和费-托法用的富CO气的生产。
已发现在自热转化器上游安排具有蒸气转化催化剂的低温转化反应器降低了蒸气与碳的临界比。蒸气转化反应器除去或减少了高级烃的含量。高级烃是由两个或多个碳原子组成的烃。蒸气转化催化剂将高级烃转化成甲烷、一氧化碳、二氧化碳和氢的混合物。
低温蒸气转化反应器可以是绝热预转化器或加热的预转化器，例如以催化的热交换器盘管的形式，如在欧洲专利公开855,366号中叙述的。从低温蒸气转化反应器得到的流出物流出口温度不高于600℃。
因此，本发明提供一种用于在自热转化器中通过烃进料的催化自热转化制备富氢和/或富一氧化碳气的方法，该方法还包括的步骤：
(a)将烃进料通过含蒸气转化催化剂的第一反应器以基本上除去在烃进料中的高级烃；
(b)将第一反应器的流出物通入自热转化器中；和
(c)从自热转化器中取出富氢和/或富一氧化碳的产品气。
作为本发明的一个优点，将可以在比当使用未转化进料物流作自热转化器进料时更低的蒸气与碳比值下操作自热反应器。
作为第二优点，当它不含高级烃时可以预热ATR的进料气到较高温度。其结果是方法的耗氧较低。
本发明对伴生气的蒸气转化尤其有效。伴生气是采油期间产生的天然气。因为运送伴生气不经济，所以通常这种气体在钻井被火炬燃烧。伴生气有高含量的高级烃。
总结而言，本发明提供了以下技术方案：
一种用于在自热转化器中通过含高级烃的烃进料的催化自热转化制备富氢和/或富一氧化碳气的方法，该方法还包括步骤：
(a)将烃进料通过含蒸气转化催化剂的第一反应器除去或减少在烃进料中的高级烃含量；
(b)将从第一反应器得到的流出物通入自热转化器中；和
(c)从自热转化器中取出富氢和/或富一氧化碳的产品气。
一种实施方案是其中烃进料是天然气和/或伴生气。
一种实施方案是其中第一反应器以绝热方式进行操作。
一种实施方案是其中第一反应器的出口温度是600℃以下。
实例1
试验装置由用于往ATR反应器提供进料的系统、ATR反应器和用于产品气后处理的设备所组成。
进料物流由天然气、蒸气、氧、氢和任选的丁烷组成。天然气的组成列于表2中。将所有气体压缩到操作压力和预热到操作温度。天然气在加入ATR反应器之前经脱硫。进料被混合成两股物流并送入ATR的燃烧炉中，第一股进料物流含天然气、氢、蒸气和任选的丁烷。这一进料物流被加热到500℃。另一股进料物流含氧和蒸气并被加热到220℃。ATR反应器中压力是2.46MPa。最好，含蒸气的天然气在加入ATR反应器之前先通过预转化器。也在这情况下、气体物流在加入ATR反应器之前被加热到500℃。
          表2
  组成   摩尔份数％
  N2   0.42
  CO2   1.16
  CH4   94.55
  C2   2.75
  C3   0.70
  C4   0.31
  C5 +   0.11
天然气的组成。
在ATR反应器中，进行亚化学计量的燃烧和其后的催化蒸气转化及转移反应。用气相色谱法测定进、出气体组成。
在ATR反应器下游，产品气被冷却和产品气的大部分蒸气含量被冷凝。如若形成烟灰，则捕获在冷凝物中。将冷凝物进行重量分析和分光光度分析检测。
进行下述试验以证明进料气通过预转化器的影响，在一个试验中，进料气中掺入丁烷。丁烷浓度为整个烃的4.0％(体积)。
用从富蒸气侧接近蒸气与碳临界比做每个试验。用足够高的蒸气流开始试验以确保无烟灰的条件。而后逐步地减低蒸气流。让体系变成稳定。稳定后检验冷凝物中的烟灰含量。如若冷凝物中仍无烟灰，进行下一步。“无烟灰条件”词指烟灰形成可不计的条件。在蒸气与碳临界比下形成的烟灰量大约3-5ppm。
在以下所叙的试验中，碳流速是100-103Nm3/h。氢流速是2Nm3/h。蒸气流速调节到获得一定的蒸气与碳比值。氧流速调节到获得希望的操作温度并在55-58Nm3/h范围。
由于从相对小中试的热损失，绝热的ATR出口温度将比表3中所给的温度要高。大型工业装置将很接近绝热条件，因此，当严格按表3所列相同条件操作工业装置时，这种装置的出口温度将很接近表3中所给的绝热值。
                                 表3
  试验号   预转化器   丁烷掺入   O2/C   ATR出口温度   绝热的出口温度   蒸气与碳临界比
  ℃   ℃
  1.1   无   无   0.56   954   1019   0.70
  1.2   有   无   0.56   951   1011   0.64
  1.3   无   有   0.55   948   1006   0.79
在表3的试验中从ATR反应器得到的产品气组成是由气相色谱法测定的。气体组成表示于表4中。气体组成以干的摩尔百分比给出。它是当不包含蒸气时的气体组分的摩尔组成。
                     表4
  试验号   H2   N2   CO   CO2   CH4
  ％   ％   ％   ％   ％
  1.1   64.4   0.14   26.74   6.81   1.87
  1.2   65.1   0.12   25.17   6.99   2.62
  1.3   64.5   0.12   26.09   7.67   1.62
表3的试验的产品气组成(干摩尔％)
从表3可见，当进料蒸气通过预转化器时蒸气与碳的临界比减小。而且，它表明在加入ATR的进料气中提高丁烷含量导致蒸气与碳的临界比增加。这意味着若进料含有大量的高级烃，进料通过预转化器的优越性将提高。
实例2
使用与实例1相同的试验装置。在试验2和3中将乙烷和丁烷加入含天然气的进料物流中。
在下面所述的试验中碳流速为102-103Nm3/h。氢流速是3Nm3/h。蒸气流速调节到获得一定的蒸气与碳比，氧的流速调节到获得所希望的操作温度并在58-60Nm3/h之间。
                                    表5
  试验号   掺入   烃    浓度总烃的％体积   O2/C   ATR出口温度℃   绝热出口温度℃   蒸气与碳临界比
  2.1   无   0.58   1027   1109   0.33
  2.2   有   乙烷   7.2   0.58   1024   1113   0.41
  2.3   有   丁烷   5.1   0.57   1023   1118   0.47
在表5的试验中从ATR反应器得到的产品气组成表示于表6中。
                             表6
  试验号   H2   N2   CO   CO2   CH4
  ％   ％   ％   ％   ％
  2.1   62.9   0.14   31.1   4.33   1.52
  2.2   63.0   0.14   30.9   4.74   1.25
  2.3   63.3   0.21   30.5   4.71   1.25
表5的试验的产品气组成(干摩尔％)
从表5可见乙烷和丁烷的高含量导致蒸气与碳比增加。

Claims (5)

1.一种用于在自热转化器中通过含高级烃的烃进料的催化自热转化制备富氢和/或富一氧化碳气的方法，该方法还包括步骤：
(a)将烃进料通过含蒸气转化催化剂的第一反应器除去或减少在烃进料中的高级烃含量；
(b)将从第一反应器得到的流出物通入自热转化器中；和
(c)从自热转化器中取出富氢和/或富一氧化碳的产品气。
2.权利要求1的方法，其中烃进料是天然气和/或伴生气。
3.权利要求1或2的方法，其中第一反应器以绝热方式进行操作。
4.权利要求1或2的方法，其中第一反应器的出口温度是600℃以下。
5.权利要求3的方法，其中第一反应器的出口温度是600℃以下。
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