CN101534925A - 获得二氧化碳的方法 - Google Patents

获得二氧化碳的方法 Download PDF

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CN101534925A
CN101534925A CNA2007800426642A CN200780042664A CN101534925A CN 101534925 A CN101534925 A CN 101534925A CN A2007800426642 A CNA2007800426642 A CN A2007800426642A CN 200780042664 A CN200780042664 A CN 200780042664A CN 101534925 A CN101534925 A CN 101534925A
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乌尔里希·科斯
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Abstract

在用于获得CO2的方法中，在900～1200℃的温度和40～100巴(a)的压力下，在添加含氧气体的条件下，通过部分催化氧化，将脱硫天然气或石油伴生气自热重整而获得粗合成气，然后在75～110℃的温度和CO的50～75巴(a)的压力下，催化转化成H2和CO2，在15～100巴(a)的压力和+10～－80℃的温度下，用甲醇将CO2从所得合成气中洗涤出来，并且通过降压回收所吸收的CO2。本方法的进一步可能用途在于将所回收的CO2转化为超临界状态。

Description

获得二氧化碳的方法
技术领域
本发明涉及一种从脱除了C2+组分的脱硫天然气或石油气中回收CO2的方法，在第一反应阶段中，通过添加包含至少[以干基计算]75体积％ O2的气体，在900～1200℃的温度和40～100巴绝对的压力下，通过在裂化催化剂的固定床上部分氧化，将预热至45～75℃温度的脱硫天然气或石油气自热重整而获得粗合成气，该粗合成气包含作为主要成分[以干基计算]的55～75体积％ H2、15～30体积％ CO和5～30体积％ CO2，其中H2:CO的体积比为1.6～4，在第二反应阶段中，在至少一种固定床催化剂上，将温度为75～110℃和压力为50～75巴绝对的粗合成气中所含的CO转化成H2和CO2，在至少一个洗涤阶段中，在15～100巴绝对的压力下，用温度为+10～-80℃的甲醇，从包含至少[以干基计算]55体积％ H2的合成气中洗掉CO2，并且通过将冷的甲醇膨胀至接近大气压来回收所吸收的CO2。
背景技术
从EP-B-1 337 466，已知由N2-H2混合物催化产生NH3的方法。在900～1200℃的温度和40～100巴绝对的压力下，在裂化催化剂存在下，使天然气与主要由优选至少70体积％的O2构成的气流一起进行自热重整而获得粗合成气，该粗合成气包含[以干基计算]55～75体积％ H2、15～30体积％ CO和5～30体积％ CO2，其中H2:CO的体积比为1.6～4。通过催化转化，将从自热重整器中引出的冷却的粗合成气中的CO内容物转化为H2，从而所形成的合成气包含至少[以干基计算]50体积％ H2和不超过8体积％ CO。在多阶段气体洗涤中，将CO2、CO和CH4从合成气中去除，其中在至少一个阶段中，添加液氮来产生N2-H2混合物，其用于氨合成中氨的催化产生。在所述气体洗涤中，CO2用温度为-58℃的甲醇来除去，并且与NH3的产生结合用来生成尿素。在N2洗涤中，将所述合成气冷却至-185℃的温度，从而首先冷凝CH4，随后冷凝CO，并且将这两种组分作为燃料气体再循环至自热重整器。
发明内容
本发明的目的是将上述的方法用于进一步的应用。
该目的的解决方案在于将回收的CO2转变为临界条件，从而为了溶剂驱动将CO2注入部分脱油的石油矿床中，或者可储存在孔隙型储层、洞穴型储层、适合作为储层的枯竭的天然气矿床或含盐的含水层中，或者能够用于羰基合成。
根据本方法的另一方面，可以将所回收的H2作为燃料全部或部分供应给燃气轮机或用于产生电能的其它装置，例如供应给燃料电池，其中根据本发明的进一步特征，所述H2可用高达70体积％N2稀释。
根据本发明的特定特征，由燃气轮机或用于获得电能的其它装置产生的部分机械能，用来驱动空气分离装置的压缩机和/或CO2的压缩装置；剩余部分可用作有用的能量。
下面将参考实施方案并结合附图中所示的基本流程图来对本发明做详细说明。
天然气经导管(1)供应给预处理装置(4)，其中压力为45～65巴绝对且温度为15～35℃，蒸汽经导管(2)和CH4经导管(3)供应给预处理装置(4)，在预处理装置(4)中，在具有下游ZnO床的Co-Mo催化剂床上，使所述天然气脱除硫化合物和C2+组分，并且将其预热至55～75℃的温度。经导管(5)从所述预处理装置(4)引出的气体与经导管(7)供应的氧气含量为[以干基计算]92体积％的高氧气体一起装载入自热重整器(6)，该高氧气体在经导管(9)引入空气的空气分离装置(8)中产生。在自热重整器(6)中，设置有市售NiO催化剂床，在该催化剂床上，在900～1200℃的温度和40～100巴绝对、优选40～80巴绝对的压力下，通过利用O2部分氧化，将所述天然气重整而获得包含CO、H2和CO2的粗合成气。从自热重整器(6)中经导管(10)引出的粗合成气包含[以干基计算]55～75体积％ H2、15～30体积％的CO和5～30体积％ CO2，其中H2:CO的体积比为1.6～4。在未示出的热交换器中中间冷却至25～45℃的温度的粗合成气通入填充有市售Fe-Cr催化剂床的两阶段转化器(11)中，在该两阶段转化器中，将仍包含在所述粗合成气流中的CO转化成CO2和H2，其中H2:CO2的体积比[以干基计算]为2.5～3。在穿过未示出的热交换器后，将经过转化获得并经导管(12)引出的合成气流引入两阶段物理气体洗涤装置(13)中，所述合成气流包含[以干基计算]至少65体积％H2和不超过8体积％CO。在气体洗涤装置(13)的第一阶段(14)中，在40～80巴绝对的压力下，借助温度为-20～-70℃的甲醇来吸收CO2。在气体洗涤装置(13)的第二阶段(15)中，借助在空气分离装置(8)中回收的并且经导管(16)装载入第二阶段(15)中的液氮来吸收脱除CO2时残留在合成气流中的杂质CO、CH4和Ar。为了从甲醇中去除吸收的CO2以及从N2中去除吸收的CO、CH4和Ar，将所述甲醇和N2膨胀至接近大气压。将回收的CO2经导管(17)供应给装置(18)，在该装置(18)中通过升高压力和温度使CO2变成超临界条件，并且经导管(19)将其注入部分脱油的石油矿床中用于溶剂驱动。包含CO、CH4和Ar的气流作为燃料气体经导管(20)再循环至自热重整器(6)。在气体洗涤装置(13)的第一阶段(14)中吸收CO2的过程中得到的H2作为燃料经导管(21)流入燃气轮机(22)的燃烧室中。
参照附图中所示的基本流程图，采用本发明方法的具体实施方案获得的有关物质量、温度、压力和气流组成的数据列于下表中。
 
导管编号 1 5 10 12 17 20 21
量(t/h) 92 263 336 400 0.044 0.01 49.8
温度(℃) 25 65 95 32 40 40 209
压力(巴绝对) 55 61 60 57 110 58 30～54
组成体积％[以干基计算]CH4                91.3 27.0 1.8 2.0 - 2.0 0.8
C2H6 5.8 - - - - - -
CO - 1.6 10.6 1.1 0.1 1.1 1.9
CO2 1.9 0.6 7.1 16.7 99.6 16.7 0.5
Ar - - 0.3 0.5 - 0.5 0.9
H2 - 3.2 38.7 47.5 0.2 47.5 92.5
N2 1.0 0.3 0.4 2.3 0.1 2.3 4.2
H2O - 67.3 41.1 29.9 - - -
对于气体洗涤(13)，采用公知的
Figure A200780042664D0007093510QIETU
方法，其中在第一阶段(14)中用温度为-58℃的甲醇来吸收CO2。在气体洗涤(13)的第二阶段(15)中，首先将合成气的温度降至-185℃的值，从而将CH4冷凝、分离及与以同样方式分离的CO和Ar一起再循环到自热重整器(3)中作为燃料气体。
利用本发明可实现的优点特别在于：
-阻止了CO2的排放，特别是出于生态原因，
-回收超临界CO2的方法能够直接就地用于可能有石油的地方为溶剂驱动而大量脱油的石油矿床，
-在许多可能有石油的地方，石油开采中获得的石油气能够直接就地加工，并且所产生的气体组分能够在该工艺内部利用。

Claims (6)

1.一种从脱除了C2+组分的脱硫天然气或石油气中回收CO2的方法，在第一反应阶段中，通过添加包含至少[以干基计算]75体积％ O2的气体，在900～1200℃的温度和40～100巴绝对的压力下，通过在裂化催化剂的固定床上部分氧化，将预热至45～75℃的温度的脱硫天然气或石油气自热重整而获得粗合成气，该粗合成气包含作为主要成分[以干基计算]的55～75体积％ H2、15～30体积％ CO和5～30体积％ CO2[以干基计算]，其中H2:CO的体积比为1.6～4，在第二反应阶段中，在至少一种固定床催化剂上将温度为75～110℃和压力为75～50巴绝对的粗合成气中所含的CO转化成H2和CO2，在至少一个洗涤阶段中，在15～100巴绝对的压力下，用温度为+10～-80℃的甲醇，从包含至少55体积％H2[以干基计算]的合成气中洗掉CO2，并且通过将冷的甲醇膨胀至接近大气压来回收所吸收的CO2，其特征在于，将所回收的CO2转变成超临界条件。
2.通过根据权利要求1所述的方法回收的CO2用于溶剂驱动部分脱油的石油矿床，或者用于储存于孔隙型储层、洞穴型储层、枯竭的天然气矿床和含盐的含水层中，或者用于羰基合成的用途。
3.根据权利要求1所述的方法，其特征在于，将所回收的H2作为燃料供应给燃气轮机和/或用于产生电能的其它装置，例如供应给燃料电池。
4.根据权利要求3所述的方法，其特征在于，用70体积％ N2对所回收的H2进行稀释。
5.根据权利要求3和4中任一项所述的方法，其特征在于，利用由燃气轮机产生的部分机械能来驱动空气分离装置的压缩机。
6.根据权利要求3至4中任一项所述的方法，其特征在于，利用由燃气轮机产生的部分机械能来驱动用于CO2的压缩机。
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