CN111974208A - 一种用于去除工艺废气中的一氧化二氮的方法 - Google Patents
一种用于去除工艺废气中的一氧化二氮的方法 Download PDFInfo
- Publication number
- CN111974208A CN111974208A CN202010428799.XA CN202010428799A CN111974208A CN 111974208 A CN111974208 A CN 111974208A CN 202010428799 A CN202010428799 A CN 202010428799A CN 111974208 A CN111974208 A CN 111974208A
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- Prior art keywords
- reducing agent
- nitrous oxide
- shaped catalyst
- monolith
- monolith shaped
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 title claims abstract description 78
- 238000000034 method Methods 0.000 title claims abstract description 57
- 239000001272 nitrous oxide Substances 0.000 title claims abstract description 23
- 239000002912 waste gas Substances 0.000 title claims description 4
- 239000003054 catalyst Substances 0.000 claims abstract description 84
- 239000007789 gas Substances 0.000 claims abstract description 37
- 239000003638 chemical reducing agent Substances 0.000 claims abstract description 35
- 230000003647 oxidation Effects 0.000 claims abstract description 15
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 15
- 238000000354 decomposition reaction Methods 0.000 claims abstract description 9
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical group N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 92
- 229910021529 ammonia Inorganic materials 0.000 claims description 46
- 239000010457 zeolite Substances 0.000 claims description 11
- 229910021536 Zeolite Inorganic materials 0.000 claims description 10
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 10
- 229910052751 metal Inorganic materials 0.000 claims description 9
- 239000002184 metal Substances 0.000 claims description 9
- 229910052802 copper Inorganic materials 0.000 claims description 7
- 229910052748 manganese Inorganic materials 0.000 claims description 7
- 229910052763 palladium Inorganic materials 0.000 claims description 7
- 229910052742 iron Inorganic materials 0.000 claims description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical group C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 6
- 239000000203 mixture Substances 0.000 claims description 5
- 229930195733 hydrocarbon Natural products 0.000 claims description 4
- 150000002430 hydrocarbons Chemical class 0.000 claims description 4
- 229910052759 nickel Inorganic materials 0.000 claims description 4
- 229910052697 platinum Inorganic materials 0.000 claims description 4
- 229910052725 zinc Inorganic materials 0.000 claims description 4
- 238000010531 catalytic reduction reaction Methods 0.000 claims description 3
- 239000011248 coating agent Substances 0.000 claims description 3
- 238000000576 coating method Methods 0.000 claims description 3
- 239000004215 Carbon black (E152) Substances 0.000 claims description 2
- 229910052878 cordierite Inorganic materials 0.000 claims description 2
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 claims description 2
- 239000002243 precursor Substances 0.000 claims description 2
- 229910052720 vanadium Inorganic materials 0.000 claims description 2
- 229960001730 nitrous oxide Drugs 0.000 abstract 4
- 235000013842 nitrous oxide Nutrition 0.000 abstract 1
- 229910002089 NOx Inorganic materials 0.000 description 24
- 238000006243 chemical reaction Methods 0.000 description 20
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 19
- 229910017604 nitric acid Inorganic materials 0.000 description 14
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 13
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 12
- 238000004519 manufacturing process Methods 0.000 description 9
- 238000002156 mixing Methods 0.000 description 7
- 238000006722 reduction reaction Methods 0.000 description 7
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 6
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 description 6
- 239000000243 solution Substances 0.000 description 6
- 230000015572 biosynthetic process Effects 0.000 description 5
- 238000011144 upstream manufacturing Methods 0.000 description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- 230000003197 catalytic effect Effects 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- MGWGWNFMUOTEHG-UHFFFAOYSA-N 4-(3,5-dimethylphenyl)-1,3-thiazol-2-amine Chemical compound CC1=CC(C)=CC(C=2N=C(N)SC=2)=C1 MGWGWNFMUOTEHG-UHFFFAOYSA-N 0.000 description 3
- 239000006096 absorbing agent Substances 0.000 description 3
- 238000010521 absorption reaction Methods 0.000 description 3
- 239000005431 greenhouse gas Substances 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 230000003068 static effect Effects 0.000 description 3
- PAWQVTBBRAZDMG-UHFFFAOYSA-N 2-(3-bromo-2-fluorophenyl)acetic acid Chemical compound OC(=O)CC1=CC=CC(Br)=C1F PAWQVTBBRAZDMG-UHFFFAOYSA-N 0.000 description 2
- 238000002485 combustion reaction Methods 0.000 description 2
- 238000009434 installation Methods 0.000 description 2
- 230000003389 potentiating effect Effects 0.000 description 2
- 238000005979 thermal decomposition reaction Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- BFNBIHQBYMNNAN-UHFFFAOYSA-N ammonium sulfate Chemical compound N.N.OS(O)(=O)=O BFNBIHQBYMNNAN-UHFFFAOYSA-N 0.000 description 1
- 229910052921 ammonium sulfate Inorganic materials 0.000 description 1
- 235000011130 ammonium sulphate Nutrition 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 229940112112 capex Drugs 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 238000003421 catalytic decomposition reaction Methods 0.000 description 1
- 229910000428 cobalt oxide Inorganic materials 0.000 description 1
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- -1 dinitrogen compound Chemical class 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000002360 explosive Substances 0.000 description 1
- 239000003337 fertilizer Substances 0.000 description 1
- FEBLZLNTKCEFIT-VSXGLTOVSA-N fluocinolone acetonide Chemical compound C1([C@@H](F)C2)=CC(=O)C=C[C@]1(C)[C@]1(F)[C@@H]2[C@@H]2C[C@H]3OC(C)(C)O[C@@]3(C(=O)CO)[C@@]2(C)C[C@@H]1O FEBLZLNTKCEFIT-VSXGLTOVSA-N 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 238000005949 ozonolysis reaction Methods 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 239000003870 refractory metal Substances 0.000 description 1
- 238000003303 reheating Methods 0.000 description 1
- 239000005437 stratosphere Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000002341 toxic gas Substances 0.000 description 1
Classifications
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Abstract
本发明涉及一种用于在轴向流反应器中去除工艺废气中所含的一氧化二氮(N2O)的方法,其包括以下步骤:(a)向工艺废气中添加一定量的还原剂;(b)在第一阶段中,使与还原剂混合的工艺废气沿轴向流动方向通过第一整料成型催化剂,以提供具有减少量的一氧化二氮和残留量的还原剂的气体,该第一整料成型催化剂对于一氧化二氮经由还原剂的分解反应是有活性的;和(c)在第二阶段中,使具有减少量的一氧化二氮以及残留量的还原剂的气体沿轴向流方向通过第二整料成型催化剂,该第二整料成型催化剂对于残留量的还原剂的氧化是有活性的。
Description
技术领域
本发明涉及一种用于联合去除工艺废气中的氮氧化物(一氧化二氮,N2O)的方法。
发明背景
N2O是一种强大的温室气体,因此在具有CO2市场的地区与成本相关。因此,N2O的去除需要尽可能经济高效地进行。
硝酸生产是已知具有N2O排放的工业。由于在催化反应器下游的冷点中存在形成硝酸铵的风险,因此硝酸生产也对于来自N2O去除过程中的氨(NH3)逸出具有非常严格的要求。逸出要求通常为5ppm或更低至3甚至2ppm。
N2O的去除需要尽可能经济高效地进行。
硝酸(HNO3)主要用于制造化肥和***。
硝酸按照德国化学家威廉·奥斯特瓦尔德(Wilhelm Ostwald)的奥斯特瓦尔德工艺生产。在此工艺中,氨(NH3)被氧化为一氧化氮(NO)。一氧化氮被氧化成二氧化氮(NO2),二氧化氮被吸收在水中形成硝酸。该过程是加压的,并且废气中包含NOx和N2O,除此之外非常干净。
但是,将NH3氧化为NO并不是100%选择性的,这意味着除了所期望的NO之外,还会形成一定量的氮(N2)和二氮化物(一氧化二氮,N2O)。
取决于氧化条件,即NH3燃烧过程中的常用(prevailing)压力、温度和流入速度,以及催化剂的类型和老化状态,通常每公吨HNO3会形成约4-15kg的N2O。这导致工艺废气中N2O浓度通常约为500-2000ppm(体积)。
在水中吸收二氧化氮(NO2)以形成硝酸时不会吸收所形成的N2O。因此,N2O随HNO3生产的工艺废气被排出。
由于安装在吸收塔下游以减少NO和NO2残留含量(二者统称为NOx)的DeNOx级通常不会降低N2O含量,因此N2O最终会排放到大气中。
由于N2O是强效的温室气体,其效果是CO2的300倍左右,并且硝酸设备目前代表了N2O气体的单一最大工业工艺源,N2O对平流层中的臭氧分解和温室效应做出了巨大贡献。因此,出于环境保护的原因,越来越需要用于减少硝酸生产和其他工业过程中N2O排放问题的技术性解决方案。
降低HNO3设备中N2O排放的已知可能方法可大致分为三类:
第一解决方案:首先防止N2O的形成。这需要对铂丝网(gauze)进行改进以减少N2O的形成。可替代材料可以用作氨氧化催化剂。例如,钴氧化物不会产生大量的N2O副产物,但对NO的生成选择性较低。
第二解决方案:一氧化二氮一旦形成,便会在氨氧化丝网的出口与吸收塔的入口之间的任何位置被去除。在第二解决方案的方法中,选择的位置直接在温度最高的丝网之后。大多数技术都采用粒状形式的催化剂,这些催化剂是松散的或封闭在由耐热金属丝制成的笼子中,而有些则使用蜂窝状形式的催化剂。
第三解决方案:通过催化分解为N2和O2或通过化学还原剂进行催化还原,从吸收塔下游的工艺废气中除去N2O。设置第三减排步骤的最佳位置通常位于紧接膨胀涡轮机上游的吸收塔下游的最热位置。已知的解决方案是使用包括铁沸石的粒状催化剂,铁沸石以径向或水平流过催化剂床的方式布置,以将压降保持在可接受的水平。这通常需要更大的反应器。
已知第三催化剂单元通常使用两个床:第一床用于除去大量的N2O,然后添加还原剂;第二床用于除去剩余的N2O。结果是导致具有两个径向流动床和内部计量添加还原剂的反应器,其非常大且复杂。根据本发明,能够使用相同的具有两个床和床间内部计量添加还原剂的设置,但是其更简单且更小,从而降低总体复杂性和成本。
已知第三催化剂单元也可以仅具有一个床,该床具有组合的NOx和N2O的去除,其中还原剂被添加到第三反应器的上游。通过使用静态混合器的已知方法或仅通过充分的混合时长即可实现充分的混合。
为了获得低的N2O排放量和低的NH3逸出量,需要在气体中高效混合NH3并且需要较大的催化剂量,以使反应发生。
在具有径向或水平流动的反应器中,不可能制备一个具有不同于本发明的催化剂类型底层。在具有径向或水平流的反应器中,它必须是单独的床,这增加了反应器的尺寸和成本。
通常,借助于包含铁沸石的催化剂颗粒以在制备硝酸的尾气中除去N2O。
反应器设计成径向或水平流过催化剂床,以将压降保持在可接受的水平。这通常需要更大的反应器体积。
这是由于在下游的冷点或在堆中可能形成硝酸铵,还原剂氨的逸出对硝酸生产造成安全隐患。因此,对氨逸出的要求通常非常严格。
使用烃作为还原剂的工艺通常具有较低的活性,并会发生用过的烃与部分燃烧产物(例如CO)一起大量逸出的现象。在此类过程中,经常用作还原剂的甲烷本身就是强效的温室气体,因此在一定程度上抵消了N2O排放量的减少。同时,一氧化碳是有毒气体,因此不期望被排放到大气中。
为了获得低的N2O排放和低的还原剂逸出,需要在气体中高效混合还原剂,同时需要更大的催化剂量以进行反应。
在已知的具有径向或水平流动方向的反应器中,不可能安装具有针对氨逸出的催化剂的底层。
当使用氨作为还原剂时,为了使N2O分解反应有效发生并使氨的逸出低于5ppm或更低,在这些反应器中需要大量额外的催化剂。
发明内容
在本发明的方法中,添加了另外的催化阶段,其中还原剂例如氨被氧化。
这允许在除去N2O中使用较少量的活性催化剂,并且允许使用总量更小的催化剂,这导致反应器更紧凑和CAPEX更低。
已知的用于减少N2O的方法在第三设备中使用粒状催化剂。这些催化剂通常安装在径向流转换器中,以保持低的压降。这种径向流转换器大而笨重,并且在设计方面有多种限制。由于反应器通常是加压的,因此反应器的成本随着反应器直径的增加而显著增加。这是加压容器众所周知的效果。
本发明提供了一种用于在轴向流反应器中去除工艺废气中所含的一氧化二氮(N2O)的改进方法,该方法包括以下步骤:
(a)向工艺废气中添加一定量的还原剂;
(b)在第一阶段中,使工艺废气与还原剂混合并沿轴向流方向通过第一整料成型催化剂,以提供具有减少量的一氧化二氮和残留量的还原剂的气体,该第一整料成型催化剂对于一氧化二氮与还原剂的分解反应是活性的;和
(c)在第二阶段中,使具有减少量的一氧化二氮和残留量的还原剂的气体沿轴向流方向通过第二整料成型催化剂,该第二整料成型催化剂对氧化残留量的还原剂是活性的。
术语“去除一氧化二氮(N2O)”应被理解为至少减少N2O的量。
术语“整料成型催化剂”应理解为包含或涂覆有催化活性材料的整料成型催化剂或蜂窝状催化剂。
整料成型催化剂优选在反应器内以一层或多层的形式有序排列。
与使用粒状催化剂的径向流反应器的设计相比,整料成型催化剂能够实现轴向流反应器的设计,同时提供低的压降。
轴向流反应器的直径可以设计得比径向流反应器的直径小,从而可以降低反应器的成本,并可以在对安装空间要求不严格的情况下进行安装。与设计用于使用粒状催化剂的径向流反应器不同,轴向流反应器还可以水平安装,从而可以优化给定安装的空间需求。
任选地,可以在上游催化剂床中去除一部分N2O而无需注入还原剂,并且在第二下游床中去除剩余量的N2O。这种布置的目的是减少用于还原N2O的还原剂的消耗,因为已经使一些N2O在上游床中发生了热分解。
因此,在本发明的一个实施方案中,该方法还包括在步骤(a)之前使该工艺废气沿轴向流方向通过对一氧化二氮分解有活性的整料成型催化剂的步骤。
优选地,进一步的步骤包括使工艺废气通过对于一氧化二氮的热分解具有活性的整料成型催化剂,该催化剂包括金属交换的沸石,其中金属包含Fe、Co、Ni、Cu、Mn、Zn、Pd、或其混合物。
在本发明的一个实施方案中,第一整料成型催化剂包括金属交换的沸石,其中金属包含Fe、Co、Ni、Cu、Mn、Zn、Pd、或其混合物。
优选地,金属交换的沸石选自由MFI、BEA、FER、MOR、FAU、CHA、AEI、ERI和/或LTA组成的组。
最优选地,金属交换的沸石是Fe-BEA。
在一个实施方案中,第二整料成型催化剂选自V、Cu、Mn、Pd、Pt或其氧化物或其组合。
在另一个实施方案中,第二整料成型催化剂另外包含一种或多种金属交换的沸石。
在本发明的另一个实施方案中,第一整料成型催化剂和第二整料成型催化剂包括挤出的整料成型载体,优选堇青石。
在另一个优选的实施方案中,第一和/或第二整料成型催化剂以多于一个层的形式堆叠布置在反应器内部。
在又一个实施方案中,第二整料成型催化剂以区域涂层的形式布置在整料成型载体上。
在一个优选的实施方案中,还原剂是氨或其前体。
在另一个实施方案中,还原剂为烃,优选为甲烷。
在另一个优选的实施方案中,第一整料成型催化剂对于一氧化二氮经由氨的分解反应和对于NOx经由氨的选择性催化还原反应均具有活性。
发明详述
在下面根据对其具体实施方案的详细描述,进一步说明了本发明。
在工艺废气再加热之后但在膨胀器之前,在吸收塔下游的硝酸工艺中进行根据本发明的方法。将氨注入到气流中并混合到废气中。在第一阶段,将与氨混合的废气引入安装了第一整料成型催化剂的反应器。在第一阶段中,N2O与氨根据以下反应:
3N2O+2NH3→4N2+3H2O
NOx通过众所周知的SCR反应进行反应,这也需要氨。在第一阶段中,催化剂的量应使得在第一阶段后,气体中残留的NOx和N2O明显减少,并且NH3逸出约为10ppm。
随后使该废气进入包含第二整料成型催化剂的第二阶段,在第二阶段中,大部分逸出的氨被氧化,从而形成N2或NOx。
在第二阶段中由NH3氧化而形成的任何NOx都不成问题,因为来自第一阶段的NOx排放量非常低(几乎为0ppm),从第一阶段逸出到第二阶段的NH3保持在如此低的水平,以至于选择性降低仍只会导致有限的NOx排放。假设从第一阶段逸出10ppm氨,第二阶段对氨到NOx的选择性为100%,则在第二阶段仍仅形成10ppm NOx。
温度通常在380-550℃的范围内。压力通常在4-12bar g的范围内,但可以更高或更低。更高的压力增加了NOx和N2O在第一阶段中的转化活性,并且增加了NH3在第二阶段中的转化。
第一阶段和第二阶段的正常时空速度取决于温度、压力和所需的性能,但通常在第一阶段为10000-40000h-1,在第二阶段为80000-120000h-1。
通常,在第一阶段中使用的第一整料成型催化剂的催化剂量比第二阶段中的催化剂量大3-5倍。
在一个实施方案中,第二阶段包括对NH3氧化具有活性的催化剂以及对SCR反应具有活性的催化剂。第二整料成型催化剂具有与第一整料成型催化剂相似的组成,其中添加了对NH3氧化具有活性的催化剂,例如Cu、Mn、Pd或Pt。从而,如果NOx是通过NH3的氧化而形成的,则可以通过使NOx与尚未转化的NH3在对于SCR反应为活性的催化剂上进行反应来去除NOx,从而进一步减少了NOx的排放。
如果在第二阶段中还存在与第一阶段相似的催化剂,则还原N2O的反应也可在第二阶段中继续进行。
第二阶段可以如下任选地进行,其中第二整料成型催化剂以区域涂层的形式布置在整料成型载体上。
例如,当将常规装置与本发明第一和第二阶段的操作相比时,则可在催化剂量显著降低的情况下保持N2O的还原反应活性。第一阶段可以在例如11ppm的氨逸出下操作,然后使氨氧化的第二阶段将氨逸出显著降低到低于5ppm的水平。结果通常是,第一阶段中的催化剂量可以减少约40%,而第二阶段通常需要的催化剂量比第一阶段中催化剂床中节省的催化剂量少50%,导致本发明的总催化剂量减少超过20%。
另外,通过随后从第一阶段去除大部分的逸出氨,大大降低了将氨与废气混合的要求。
在常规反应器中,重要的是要提供NH3与废气的高效混合,以获得高的NOx和N2O去除率以及低的氨逸出。当NH3与废气的混合不充分时,会出现NH3不足的区域,这意味着这些区域中的NOx和N2O转化会受到影响,并且还会有NH3过多的区域,这意味着来自这些区域的氨逸出会更高。为了获得NOx和N2O的高转化率以及低的NH3逸出,需要非常好的混合。通常需要静态混合器,这会导致额外的成本和设备中的压降。
通过本发明,可以将稍微更高量的NH3计量加入废气中,使得来自第一阶段的平均NH3逸出量为例如10ppm而不是2ppm(如果2ppm是避免在催化NOx和N2O转化下游的冷点中形成硫酸铵的要求)。
在第二阶段中,NH3的氧化与NOx和N2O的存在无关。此外,NH3的氧化约为一级反应,因此在给定的催化剂量下,氨的氧化在第二阶段中基本恒定。这意味着来自第一阶段的更大的NH3逸出量将导致在第二阶段中除去更多的NH3(转化百分率大致相同),并且来自第二阶段的总逸出量将变小且变化较小。
具体实施方式
使温度为450℃,NOx浓度为285ppm和N2O浓度为1000ppm的工艺气体通过固定量的含铁沸石的第一整料成型催化剂。将各种量的氨混合到气体中。通过使用静态混合器和催化转化器上游的长流动距离(long flow distance)来将氨非常好地混合到气体中。
当加入915ppm氨时,N2O转化率达到92%,导致氨逸出为26.8ppm。所有NOx被除去。减少氨的剂量以得到低于2ppm的氨逸出,这是硝酸工业所要求的,这导致氨的剂量为643ppm。降低的氨量导致降低的N2O转化率,使得该转化率仅为65%。将催化剂量增至两倍仍不足以得到仅有2ppm氨逸出的92%的N2O转化率。
与之相比,在第一催化剂之后,以对应于第一催化剂的初始量的仅23%的量添加第二催化剂(该第二催化剂包含对氨的氧化是有活性的金属氧化物),上述26.8ppm的氨逸出被降低至低于2ppm的氨逸出。
这清楚地说明了当使用对氨的氧化是有活性的第二催化剂来降低来自催化反应器的氨逸出时,所需的催化剂总量显著减少。
Claims (14)
1.一种用于在轴向流反应器中去除工艺废气中所含的一氧化二氮N2O的方法,该方法包括以下步骤:
(a)向工艺废气中添加一定量的还原剂;
(b)在第一阶段中,使与还原剂混合的工艺废气沿轴向流方向通过第一整料成型催化剂,以提供具有减少量的一氧化二氮和残留量的还原剂的气体,所述第一整料成型催化剂对于一氧化二氮与还原剂的分解是有活性的;和
(c)在第二阶段中,使具有减少量的一氧化二氮以及残留量的还原剂的气体沿轴向流方向通过第二整料成型催化剂,所述第二整料成型催化剂对于残留量的还原剂的氧化是有活性的。
2.根据权利要求1所述的方法,其还包括在步骤(a)之前使所述工艺废气沿轴向流方向通过对于一氧化二氮的分解有活性的整料成型催化剂的步骤。
3.根据权利要求2所述的方法,其中对于一氧化二氮的分解有活性的整料成型催化剂包括金属交换的沸石,其中所述金属包括Fe、Co、Ni、Cu、Mn、Zn、Pd、或其混合物。
4.根据权利要求1至3中任一项所述的方法,其中所述第一整料成型催化剂包括金属交换的沸石,其中所述金属包括Fe、Co、Ni、Cu、Mn、Zn、Pd、或其混合物。
5.根据权利要求3或4所述的方法,其中所述金属交换的沸石选自由MFI、BEA、FER、MOR、FAU、CHA、AEI、ERI和/或LTA组成的组。
6.根据权利要求3至5中任一项的方法,其中所述金属交换的沸石是Fe-BEA。
7.根据权利要求1至6中任一项所述的方法,其中所述第二整料成型催化剂选自V、Cu、Mn、Pd、Pt、其氧化物或其组合。
8.根据权利要求1至7中任一项所述的方法,其中所述第一整料成型催化剂和第二整料成型催化剂包括挤出的整料成型载体。
9.根据权利要求8所述的方法,其中所述挤出的整料成型载体由堇青石组成。
10.根据权利要求1至9中任一项所述的方法,其中所述第一整料成型催化剂以多于一个层的形式堆叠布置在所述反应器中。
11.根据权利要求1至10中任一项所述的方法,其中将所述第二整料成型催化剂作为区域涂层布置在整料成型载体上。
12.根据权利要求1-11中任一项所述的方法,其中所述还原剂是氨、氨的前体、或烃。
13.根据权利要求12所述的方法,其中所述还原剂是甲烷。
14.根据权利要求12所述的方法,其中所述第一整料成型催化剂对于一氧化二氮经由氨的分解反应以及对于NOx经由氨的选择性催化还原反应均有活性。
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