CN110312563A - 用于去除工业设备的废气中包含的硫氧化物和氮氧化物的方法 - Google Patents
用于去除工业设备的废气中包含的硫氧化物和氮氧化物的方法 Download PDFInfo
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- CN110312563A CN110312563A CN201880012301.2A CN201880012301A CN110312563A CN 110312563 A CN110312563 A CN 110312563A CN 201880012301 A CN201880012301 A CN 201880012301A CN 110312563 A CN110312563 A CN 110312563A
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- Prior art keywords
- exhaust gas
- oxysulfide
- bag
- scr
- ammonia
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- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 title claims abstract description 40
- 239000007789 gas Substances 0.000 title claims abstract description 39
- 238000000034 method Methods 0.000 title claims abstract description 35
- 229910052815 sulfur oxide Inorganic materials 0.000 title claims description 9
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 title claims description 6
- 239000011593 sulfur Substances 0.000 title claims description 5
- XTQHKBHJIVJGKJ-UHFFFAOYSA-N sulfur monoxide Chemical compound S=O XTQHKBHJIVJGKJ-UHFFFAOYSA-N 0.000 claims abstract description 20
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- WWILHZQYNPQALT-UHFFFAOYSA-N 2-methyl-2-morpholin-4-ylpropanal Chemical compound O=CC(C)(C)N1CCOCC1 WWILHZQYNPQALT-UHFFFAOYSA-N 0.000 claims description 14
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 12
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- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 7
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- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 6
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- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 5
- 239000011572 manganese Substances 0.000 claims description 5
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- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 4
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- GNTDGMZSJNCJKK-UHFFFAOYSA-N divanadium pentaoxide Chemical compound O=[V](=O)O[V](=O)=O GNTDGMZSJNCJKK-UHFFFAOYSA-N 0.000 claims description 4
- 238000007254 oxidation reaction Methods 0.000 claims description 4
- UIIMBOGNXHQVGW-UHFFFAOYSA-M Sodium bicarbonate Chemical compound [Na+].OC([O-])=O UIIMBOGNXHQVGW-UHFFFAOYSA-M 0.000 claims description 3
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- 229910052763 palladium Inorganic materials 0.000 claims description 3
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- 229910052697 platinum Inorganic materials 0.000 claims description 3
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims description 3
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- 241000790917 Dioxys <bee> Species 0.000 claims 1
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- 239000002131 composite material Substances 0.000 claims 1
- 229910000765 intermetallic Inorganic materials 0.000 claims 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims 1
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- 238000006243 chemical reaction Methods 0.000 description 3
- 239000003795 chemical substances by application Substances 0.000 description 3
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 3
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- 239000000908 ammonium hydroxide Substances 0.000 description 2
- BFNBIHQBYMNNAN-UHFFFAOYSA-N ammonium sulfate Chemical compound N.N.OS(O)(=O)=O BFNBIHQBYMNNAN-UHFFFAOYSA-N 0.000 description 2
- 229910052921 ammonium sulfate Inorganic materials 0.000 description 2
- 235000011130 ammonium sulphate Nutrition 0.000 description 2
- 238000003763 carbonization Methods 0.000 description 2
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- 239000003546 flue gas Substances 0.000 description 2
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- 125000004435 hydrogen atom Chemical class [H]* 0.000 description 2
- 230000002779 inactivation Effects 0.000 description 2
- 239000002905 metal composite material Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
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- 229910052717 sulfur Inorganic materials 0.000 description 2
- 238000011144 upstream manufacturing Methods 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 1
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
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- 239000004202 carbamide Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 239000000112 cooling gas Substances 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 230000009977 dual effect Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-M hydrogensulfate Chemical compound OS([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-M 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
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- 239000003949 liquefied natural gas Substances 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
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- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical compound [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 description 1
- SOQBVABWOPYFQZ-UHFFFAOYSA-N oxygen(2-);titanium(4+) Chemical group [O-2].[O-2].[Ti+4] SOQBVABWOPYFQZ-UHFFFAOYSA-N 0.000 description 1
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- 229910000030 sodium bicarbonate Inorganic materials 0.000 description 1
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- 239000010959 steel Substances 0.000 description 1
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- -1 sulphur compound Chemical class 0.000 description 1
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- 229910001930 tungsten oxide Inorganic materials 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- 239000002912 waste gas Substances 0.000 description 1
Classifications
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- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
Abstract
本发明涉及用于通过利用SOx吸附和氨‑SCR来清洁一个过滤单元的废气的方法，该废气含有硫氧化物(SOx)、氮氧化物(NOx)和颗粒物质，该过滤单元特别是具有一个或多个催化织物过滤器组件的过滤袋室。
Description
发明领域
本发明涉及一种用于通过使用SOx吸附和氨-SCR来清洁一个过滤单元，特别是具有一个或多个催化织物过滤器组件的过滤袋室(filter bag house)的包含硫氧化物(SOx)、氮氧化物(NOx)和颗粒物质的废气的方法。
发明背景
选择性催化还原(SCR)主要是将氮氧化物(NOx)转化为N2和H2O的手段。将还原剂(通常为无水氨或氨水)添加到烟道气或废气的流中，然后其被吸附到催化剂上。
一个公知的问题是使用氨作为还原剂的SCR烟道气在低温下会形成硫酸氢铵(ABS)，导致SCR催化剂失活和下游设备产生ABS粘层。
由负载在二氧化钛上的氧化钒组成的SCR催化剂是众所周知的并且通常用于固定应用中。这些催化剂任选地用钨和/或钼氧化物或各种贵金属(例如钯和铂)促进。SCR催化剂最常用于涂覆在整料式载体(monolithicsubstrate)上。其他已知的SCR催化剂包括用铜和/或铁促进的沸石。
当气体接触SCR催化剂时发生NOX还原反应。将氨或诸如尿素的前体注入并与SCR催化剂上游的气体混合。
使用无水氨或氨水进行选择性催化还原过程的化学计量反应的化学方程式如下所示：
4NO+4NH3+O2→4N2+6H2O
2NO2+4NH3+O2→3N2+6H2O.
NO+NO2+2NH3→2N2+3H2O.
来自某些工业过程的废气除NOx外还含有SOx。
这种过程的一个例子是煤炭碳化以生产钢铁工业的焦炭。焦炉煤气(COG)是煤炭碳化的有价值的副产品。COG是潜在原料，其通过COG的部分氧化用于氢分离、甲烷富集、甲醇生产和合成气生产。它还可以有效地用于发电和生产液化天然气。
COG中典型的SOx含量为150mg/Nm3–180mg/Nm3。
发明内容
为了适合作为一种有价值的废气，COG以及其他含SOx和NOx的废气必须通过将杂质任选连同也包含在废气中的灰尘或颗粒物质去除来进行清洁。
如上所述，具有高SOX含量的气体的氨-SCR脱氮过程中的问题在于形成硫酸氢铵。通过下面的反应方案，SO3与氨反应产生硫酸铵((NH4))2SO4)和ABS(NH4HSO4)：
2SO2+O2→2SO3
2NH3+SO3+H2O→(NH4))2SO4
NH3+SO3+H2O→NH4HSO4
ABS在SCR反应器入口处的本体露点通常为约290℃，但由于SCR催化剂的微孔结构中的毛细力，观察到的露点更高。
一些SCR催化剂，如基于钒的催化剂，对来自硫酸铵盐，尤其是硫酸氢铵的污染特别敏感，该硫酸铵盐在催化剂的孔结构中在更低温度下冷凝，由此物理地阻塞该孔并使催化剂失活。
避免在低于硫酸氢铵露点下进行废气清洁的一种方法是在冷却气体之前进行SCR和SOx吸附。
在另一方面，出于降低的能量需求和分离包含在某些废气中的有价值的有机化合物(如苯、甲苯和二甲苯)的可能性，当在SCR反应之前冷却来自生产设备的热废气时，在低于硫酸氢铵的露点的低温下进行SCR操作是可取的。
处理此问题的另一方法是定期在高温度下操作SCR，其中从催化剂中释放硫酸氢铵，且使得催化剂孔可用于催化反应。这样，催化剂被重新激活。
当在SCR操作和颗粒物质过滤中使用催化织物袋过滤器时，该过程必须在低于袋的破坏温度的操作温度下进行。通常，过滤袋仅耐受高达约240℃，这使得无法在较高温度下进行定期热处理。
本发明的基本想法是在NH3-SCR中在低于硫酸氢铵的露点下操作催化袋过滤器，并同时借助于粉状硫吸附剂去除硫氧化物和所形成的硫酸氢铵。
因此，本发明提供了一种用于去除工业设备的废气中包含的粉尘、硫氧化物和氮氧化物的方法，包括以下步骤：
将废气冷却至240至160℃的温度；
将经冷却的废气通过过滤袋室；
在过滤袋室中，向经冷却的废气中添加粉状硫氧化物吸附剂和一定量的氨或其前体形式的氮氧化物还原剂，并通过粉状硫氧化物吸附剂来吸附硫氧化物和硫酸氢铵，该硫酸氢铵通过硫氧化物与所添加的一定量的氨的一部分发生反应而形成；
将经过如此处理的废气与剩余量的氨一起通过设置在过滤袋室中的一个或多个织物过滤器组件，并将灰尘、经吸附的硫氧化物和经吸附的硫酸氢铵在一个或多个织物过滤袋组件的分散侧过滤掉；和
在一个或多个过滤袋组件的渗透侧内，通过与涂覆在织物上的SCR催化剂接触的氨的选择性催化还原来减少或去除经过滤的废气中的氮氧化物的含量。
优选地，废气通过热交换器中的间接热交换来冷却，其通常存在于大多数现有的清洁系统中以用于去除硫化合物和铵硫酸氢。这使得根据本发明的方法对于清洁系统的改型而言是有吸引力的。
当根据本发明操作该方法时，优选将包含吸附剂的碳酸氢钠粉末和作为NOx还原剂的氨一起吹到过滤袋室中。由此，硫酸氢铵和硫氧化物被吸附到吸附剂粉末上，并与灰尘和颗粒物质一起在过滤袋组件的分散侧上被过滤掉。
通常，过滤袋室将包含多个织物过滤袋组件，这些过滤袋组件以通常的方式布置在室中。
过滤袋组件可各自由单个织物过滤袋组成，其中SCR催化剂涂覆在袋的渗透侧的织物上。
在本发明的另一个实施方案中，每个过滤袋组件包括一个外过滤袋和一个或多个内过滤袋，内过滤袋分别并同心地设置在外侧管状过滤袋内。
术语“外过滤袋”是指工艺气体首先通过的过滤袋，术语“内过滤袋”是指工艺气体在通过外袋后继续通过的过滤袋。
后一实施方案具有的优点是，可以在每个过滤袋组件中的不同过滤袋上涂覆不同类型和/或量的催化剂。
施加在过滤袋上的SCR催化剂包括五氧化二钒和钛氧化物以及其它任选的钨和/或钼的氧化物。
催化活性材料可进一步包含金属和/或氧化物形式的钯或铂。
这些催化剂在通过使用NH3的SCR反应去除VOC和一氧化碳以及去除氮氧化物(NOx)二者方面都是活性的。
Pd/V/Ti催化剂是优选的催化剂，因为(i)它具有双重功能(去除NOx和去除VOC)；(ii)它具有耐硫性；和(iii)它具有比其他催化剂组合物更低的SO2氧化活性。
在本发明的另一个优选实施方案中，SCR催化剂包含负载在二氧化钛上的锰、铈和铁的氧化物的混合物。这样的SCR催化剂在大大低于190℃，例如在130℃的温度下具有足够的催化活性。由此，可以在更低温度下除去或充分减少来自SCR催化剂的氨逃逸。
存在于工艺气体中的硫氧化物吸附剂颗粒将沉积在外表面上，即织物过滤袋面向未清洁的废气的分散侧。
因此，加载到外袋和/或内袋上的催化剂被有效地保护，免受潜在的催化剂毒物，特别是存在于废气中的硫氧化物的损害。
这使得可以尤其是在该方法的低温范围内使用用铁和/或铜促进的沸石材料作为有效的SCR催化剂，包括例如Cu-SAPO-34和Cu-SSZ-13。
可用于根据本发明的方法中的另外的SCR组合物包括包含一种或多种选自由如下组成的组中的酸性沸石或沸石型组分的组合物：BEA、MFI、FAU、FER、CHA、MOR、或其与一种或多种氧化还原活性金属复合物物理混合的混合物，所述氧化还原活性金属复合物选自由如下组成的组：Cu/Al2O3、Mn/Al2O3、CeO2-ZrO2、Ce-Mn/Al2O3、及其混合物，如在美国专利9,168,517中描述的。
如上所述，根据本发明的方法非常适合于从来自焦炭生产和使用含硫燃料的再生氧化过程中的废气中去除硫氧化物和硫酸氢铵。
Claims (14)
1.用于去除工业设备的废气中包含的粉尘、硫氧化物和氮氧化物的方法，该方法包括以下步骤：
将废气冷却至240至160℃的温度；
将经冷却的废气通过过滤袋室；
在所述过滤袋室中，向经冷却的废气中添加粉状硫氧化物吸附剂和一定量的氨形式的氮氧化物还原剂，并通过粉状硫氧化物吸附剂来吸附硫氧化物和硫酸氢铵，所述硫酸氢铵通过硫氧化物与所添加的一定量的氨的一部分发生反应而形成；
将经过如此处理的废气与剩余量的氨一起通过设置在过滤袋室中的一个或多个织物过滤袋组件，并将灰尘、经吸附的硫氧化物和经吸附的硫酸氢铵在所述一个或多个织物过滤袋组件的分散侧过滤掉；和
在所述一个或多个过滤袋组件的渗透侧内，通过与涂覆在织物上的SCR催化剂接触的氨的选择性催化还原来减少或去除经过滤的废气中的氮氧化物的含量。
2.根据权利要求1所述的方法，其中经吸附的硫氧化物的主要部分由SO3组成。
3.根据权利要求1或2所述的方法，其中所述废气通过热交换进行冷却。
4.根据权利要求1至3中任一项所述的方法，其中所述粉状硫氧化物吸附剂包含碳酸氢钠。
5.根据权利要求1至4中任一项所述的方法，其中所述一个或多个过滤袋组件中的每一个由单个织物过滤袋组成。
6.根据权利要求1至4中任一项所述的方法，其中所述一个或多个过滤袋组件各自包括外过滤袋和一个或多个内过滤袋，所述内过滤袋被分别且同心地设置在所述外过滤袋内。
7.根据权利要求1至6中任一项所述的方法，其中SCR活性催化剂包括五氧化二钒和二氧化钛。
8.根据权利要求7所述的方法，其中所述SCR活性催化剂还包含钨和/或钼的氧化物。
9.根据权利要求7或8所述的方法，其中所述SCR活性催化剂还包含金属和/或氧化物形式的钯或铂。
10.根据权利要求1至6中任一项所述的方法，其中所述SCR活性催化剂包含负载在二氧化钛上的锰、铁和铈的氧化物的混合物。
11.根据权利要求1至10中任一项所述的方法，其中所述SCR活性催化剂包含用铁和/或铜促进的沸石材料。
12.根据权利要求1至10中任一项所述的方法，其中SCR活性催化剂包含一种或多种选自由以下组成的组中的酸性沸石或沸石型组分：BEA、MFI、FAU、FER、CHA、MOR、或其与一种或多种氧化还原活性金属化合物物理混合的混合物；所述氧化还原活性金属复合材料选自由以下组成的组：Cu/Al2O3、Mn/Al2O3、CeO2-ZrO2、Ce-Mn/Al2O3及其混合物。
13.根据权利要求1至12中任一项所述的方法，其中所述废气源自于使用含硫燃料的再生氧化过程。
14.根据权利要求1至12中任一项所述的方法，其中所述废气源自于焦炭生产。
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| PCT/EP2018/054646 WO2018158183A1 (en) | 2017-03-02 | 2018-02-26 | Process for the removal of sulphur oxides and nitrogen oxides contained in off-gas from an industrial plant |
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| CN113713825A (zh) * | 2021-08-31 | 2021-11-30 | 华电青岛环保技术有限公司 | 耐硫耐水的宽温脱碳催化剂及其制备方法和应用 |
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| EP4182061A1 (en) * | 2020-07-15 | 2023-05-24 | W. L. Gore & Associates, Inc. | Methods for regenerating a filter medium and cleaning flue gas |
| KR20230128513A (ko) * | 2020-12-30 | 2023-09-05 | 더블유.엘. 고어 앤드 어소시에이트스, 인코포레이티드 | 적어도 일종의 산화제를 사용하여 염 형성을 통한 연도가스 여과의 촉매 효율 향상 |
| TW202342155A (zh) * | 2022-04-01 | 2023-11-01 | 丹麥商托普索公司 | 利用選擇性催化還原來催化過濾含硫氣體之方法 |
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| KR20190121301A (ko) | 2019-10-25 |
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| TW201838708A (zh) | 2018-11-01 |
| WO2018158183A1 (en) | 2018-09-07 |
| EP3589387A1 (en) | 2020-01-08 |
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