CN110799451A - 自热氨裂化方法 - Google Patents
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- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 title claims abstract description 141
- 229910021529 ammonia Inorganic materials 0.000 title claims abstract description 69
- 238000000034 method Methods 0.000 title claims abstract description 59
- 238000005336 cracking Methods 0.000 title claims abstract description 28
- 239000007789 gas Substances 0.000 claims abstract description 66
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 60
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims abstract description 42
- 239000001257 hydrogen Substances 0.000 claims abstract description 38
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 38
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 35
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 30
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 28
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 27
- 239000001301 oxygen Substances 0.000 claims abstract description 27
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 27
- 239000003054 catalyst Substances 0.000 claims abstract description 15
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 15
- 229910001868 water Inorganic materials 0.000 claims abstract description 15
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 14
- 230000001590 oxidative effect Effects 0.000 claims abstract description 4
- 230000003647 oxidation Effects 0.000 claims description 15
- 238000007254 oxidation reaction Methods 0.000 claims description 15
- 230000003197 catalytic effect Effects 0.000 claims description 13
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 10
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 9
- 238000011084 recovery Methods 0.000 claims description 8
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- 238000006243 chemical reaction Methods 0.000 description 11
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- 239000007800 oxidant agent Substances 0.000 description 3
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- 238000004821 distillation Methods 0.000 description 2
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- 150000002431 hydrogen Chemical class 0.000 description 2
- 238000010248 power generation Methods 0.000 description 2
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- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
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- 238000002453 autothermal reforming Methods 0.000 description 1
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- 229910000510 noble metal Inorganic materials 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
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Abstract
本发明涉及用于从氨生产含有氮气和氢气的产物气体的方法,其包括以下步骤:用含有氧气的气体将氨非催化地部分氧化成含有氮气、水、一定量的氮氧化物和残余量的氨的工艺气体;通过与含镍催化剂接触,将工艺气体中至少一部分残余量的氨裂化为氢气和氮气,同时通过使工艺气体与含镍催化剂接触而与在工艺气体的裂化过程中形成的一部分氢气反应,将所述一定量的氮氧化物还原为氮气和水;以及取出含有氢气和氮气的产物气体。
Description
本发明涉及含有氮气和氢气的气体的生产。更具体地,本发明提供了一种用于生产这种气体的方法,该方法通过以下顺序进行:用含氧气体使气态氨进行非催化的部分氧化,并使部分氧化的工艺气体中含有的残余量的氨裂化为氮气和氢气产物气体。
液氨是用于产生氢气的重要来源或重要的能量载体,特别是用于在很少有或根本没有燃料源的地区产生电力。作为能量载体,液氨还可以充当一种源,以使诸如风能、太阳能和水力发电的可再生能源技术的发电量波动均匀化。氨作为能量载体的优点在于,与例如天然气或氢气相比,液氨更易于运输和存储。
为了适合用作发电的燃料,需要将氨裂化为由氢气和氮气组成的气体混合物。
在氨裂化过程中,气态氨在可逆反应中离解为氢气和氮气的混合物:
该反应是吸热的,需要热量来维持氨裂化反应。
已经发现,通过以下反应在氨的放热的非催化部分氧化中产生热量:
2NH3+3/2O2→N2+3H2O
该热量足以在随后进行氨的吸热的催化裂化时提供必要的热量。
还已经观察到,当通过与含镍催化剂接触而进行氨的裂化时,在部分氧化的气体中形成的氮氧化物被还原成氮气和水。氮氧化物通过在氨裂化反应期间形成的氢气被还原为无害的氮气和水,并且不需要用于去除裂化气体的氮氧化物的其他步骤。
另一个优点是,在根据本发明的方法不产生任何CO2的意义上,该方法允许产生不含CO2的氢气产物气体。如果将空气用作氧化剂,则少量CO2会与空气一起添加至工艺中,但由于工艺反应不生成其他CO2,因此会再次释放相同量的CO2。
根据上述观察,本发明提供了一种用于从氨生产含有氮气和氢气的产物气体的方法,其包括以下步骤:
用含有氧气的气体将氨非催化地部分氧化成含有氮气、水、一定量的氮氧化物和残余量的氨的工艺气体;
通过与含镍催化剂接触,将工艺气体中至少一部分残余量的氨裂化为氢气和氮气,同时通过使工艺气体与含镍催化剂接触而与在工艺气体的裂化过程中形成的一部分氢气反应,将所述一定量的氮氧化物还原为氮气和水;以及
取出含有氢气和氮气的产物气体。
通过本发明的方法,通过使氮氧化物与含镍催化剂接触而与氢气反应,在非催化的部分氧化步骤中产生的氮氧化物的量下降超过80%、实际上高达100%,其受热力学平衡的限制。
在本发明的一个优选实施方案中,氨的非催化的部分氧化是通过在燃烧器中在低于化学计量的氧气存在下使气态氨燃烧来进行的。
在另一个优选的实施方案中,非催化的部分氧化步骤和裂化步骤在单个反应器容器中进行。由此,来自放热的部分氧化的反应热被最佳地保存用于进行吸热的氨裂化反应。
单个反应器容器优选地被配置为自热裂化反应器,其在反应器容器的入口侧具有燃烧器,并且在燃烧器的下游具有催化剂床,其类似于图2所示的已知的自热重整反应器。
可以通过改变进入非催化的部分氧化步骤的氧气/氨进料流量比来调节与含镍催化剂接触后的平衡温度。这等效于改变λ值,该λ值是实际氧气进料流量与氨进料被完全化学计量燃烧为氮气和水所需的氧气进料流量之间的比。对于固定的氨流速,可以通过增加含有氧气的气体中的氧气浓度和/或通过增加含有氧气的气体的流速来提高平衡温度。
优选地,调节进入非催化的部分氧化步骤中的氧气/氨进料流量比,以导致在与含镍催化剂接触后测量的产物气体的平衡温度为700至1100℃。
因此,在本发明的一个实施方案中,含有氧气的气体中的氧气含量对应于λ=0.18至λ=0.30的λ值而变化,导致平衡温度为T平衡=700至1100℃。
优选地,在非催化的部分氧化步骤中使用的含有氧气的气体含有10至100vol%的氧气。
因此,含有氧气的气体的合适来源可以是烟道气、纯氧气或其混合物。
离开裂化步骤的所得产物气体混合物由氢气、氮气和水以及一定量的残余的未裂化的氨组成。
因此,在一个实施方案中,根据本发明的方法进一步包括分离进一步包含在产物气体中的未裂化的氨的步骤。
优选地,通过产物气体的水洗来进行分离步骤。在这样的分离步骤中,来自自热裂化反应器的水的主要部分将与氨一起离开分离步骤。
可以在诸如蒸馏的氨回收步骤中回收在氨分离步骤中从产物气体中分离出的一定量的氨,并且优选将回收的氨再循环到该方法中的非催化的部分氧化步骤中。同时,该氨回收步骤将清洁工艺冷凝物。
根据最终氢气/氮气产物气体的用途,可以针对预期的用途调节产物气体中氢气/氮气的摩尔比。
因此,在本发明的另一个实施方案中,该方法进一步包括在产物气体调节单元中调节产物气体的氢气/氮气摩尔比的步骤。该产物气体调节步骤可包括膜或变压吸附单元(PSA)。
本发明的一个优选实施方案进一步包括向氨进料或直接向裂化器反应器中的燃烧器添加氢气源的可能性。向氨进料添加氢气可将自动点火温度降低多达100℃,从而能够在较低的预热温度下实现自动点火,并且在正常操作期间其增加了可燃性。氢气源优选为产物气体或针对氨含量、水和/或氢气/氮气比而调节的产物气体。也可以使用来自各种公用事业来源和其他工艺的氢气。
用于裂化步骤的含有氧气的气体,例如环境空气,可以含有少量的CO2。众所周知,CO2和氨在水溶液中反应,这会导致氨回收段中的结垢和/或腐蚀。此外,如果不采取任何措施,CO2可能会在工艺中积聚。本发明的优选实施方案包括以下措施:从氧化剂中去除CO2,例如通过用NaOH溶液洗涤氧化剂;或将NaOH溶液添加到氨回收段中的蒸馏塔中,其目的是将CO2作为汽提的冷凝物中的Na2CO3而去除。
避免CO2在工艺中积聚的另一种方法是在自热氨裂化器和氨分离步骤之间包括甲烷化反应器。通过这种方法,利用从上游裂化反应器获得的氢气,将CO2转化为甲烷:
含镍或贵金属的催化剂可以催化该反应。优点是甲烷不与水溶液中的氨反应,这意味着通过甲烷化反应器中的CO2转化可以避免CO2积聚,然后生成的甲烷将与来自氨分离步骤的产物气体一起离开工艺,而不是被冷凝物夹带至回收工段。
在附图中示出了根据本发明的方法的特定实施方案,其中
图1是根据本发明的特定实施方案的氨裂化方法的示意图,其包括自热氨裂化反应器、氨分离步骤、产物气体调节和氨回收。
实施例
下表1中示出了用于氨裂化方法的工艺气体流量和组成,其对应于λ值为λ=0.21,并且在自热氨裂化反应器中与含镍催化剂接触后,所得产物气体的平衡温度为800℃。
表1
Claims (18)
1.用于从氨生产含有氮气和氢气的产物气体的方法,其包括以下步骤:
用含有氧气的气体将氨非催化地部分氧化成含有氮气、水、一定量的氮氧化物和残余量的氨的工艺气体;
通过与含镍催化剂接触,将工艺气体中至少一部分残余量的氨裂化为氢气和氮气,同时通过使工艺气体与含镍催化剂接触而与在工艺气体的裂化过程中形成的一部分氢气反应,将所述一定量的氮氧化物还原为氮气和水;以及
取出含有氢气和氮气的产物气体。
2.根据权利要求1所述的方法,其中通过使氮氧化物与含镍催化剂接触而与氢气反应,在非催化的部分氧化步骤中产生的氮氧化物的量下降超过80%至高达100%,其受热力学平衡的限制。
3.根据权利要求1或2所述的方法,其中氨的非催化的部分氧化是通过在燃烧器中在低于化学计量的含有氧气的气体存在下使气态氨燃烧来进行的。
4.根据权利要求1至3中任一项所述的方法,其中非催化的部分氧化步骤和裂化步骤在单个反应器容器中进行。
5.根据权利要求4所述的方法,其中单个反应器被配置为自热裂化反应器。
6.根据权利要求1至5中任一项所述的方法,其中调节进入非催化的部分氧化步骤中的氧气/氨进料流量比,以导致在与含镍催化剂接触后,产物气体的平衡温度为700至1100℃。
7.根据权利要求1至6中任一项所述的方法,其中含有氧气的气体中的氧气含量对应于λ值在λ==0.18至λ==0.30的之间λ值而变化,其中λ是实际氧气进料流量与所述氨被完全化学计量燃烧为氮气和水所需的氧气进料流量之间的比。
8.根据权利要求1至6中任一项所述的方法,其中含有氧气的气体含有10至100vol%的氧气。
9.根据权利要求1至8中任一项所述的方法,其进一步包括在甲烷化反应器中通过得自氨裂化步骤的氢气将CO2转化为甲烷的步骤。
10.根据权利要求1至9中任一项所述的方法,其进一步包括分离进一步包含在产物气体中的未裂化的氨的步骤。
11.根据权利要求8所述的方法,其中未裂化的氨通过水洗与产物气体分离。
12.根据权利要求10或11所述的方法,其中在氨回收步骤中回收分离出的氨,并将其再循环至非催化的部分氧化步骤。
13.根据权利要求10至12中任一项所述的方法,其包括向氨回收步骤添加NaOH。
14.根据权利要求1至13中任一项所述的方法,其进一步包括在产物气体调节单元中调节产物气体的氢气/氮气摩尔比的步骤。
15.根据权利要求1至14中任一项所述的方法,其包括向氨进料或直接向裂化反应器中的燃烧器添加氢气源。
16.根据权利要求15所述的方法,其中氢气源为氨裂化产物气体,或针对氨含量和/或氢气/氮气比进行了调节的产物气体。
17.根据权利要求15所述的方法,其中氢气源是公用事业供应或来自另一工艺。
18.根据权利要求1至17中任一项所述的方法,其包括含有氧气的气体的CO2去除洗涤。
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