CN109364713A - 一种同时脱除烟气中SO2和NOx的方法 - Google Patents
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- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 47
- 239000003546 flue gas Substances 0.000 title claims abstract description 47
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- -1 ruthenium amine Chemical class 0.000 claims abstract description 47
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- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims abstract description 20
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 18
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims abstract description 18
- 239000000908 ammonium hydroxide Substances 0.000 claims abstract description 18
- 150000003839 salts Chemical class 0.000 claims abstract description 17
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 10
- 239000007788 liquid Substances 0.000 claims abstract description 10
- 239000001301 oxygen Substances 0.000 claims abstract description 10
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 10
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 9
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- YBCAZPLXEGKKFM-UHFFFAOYSA-K ruthenium(iii) chloride Chemical group [Cl-].[Cl-].[Cl-].[Ru+3] YBCAZPLXEGKKFM-UHFFFAOYSA-K 0.000 claims description 5
- VJVWNPYNKXNTJV-UHFFFAOYSA-K [Ru+3].I(=O)(=O)[O-].I(=O)(=O)[O-].I(=O)(=O)[O-] Chemical compound [Ru+3].I(=O)(=O)[O-].I(=O)(=O)[O-].I(=O)(=O)[O-] VJVWNPYNKXNTJV-UHFFFAOYSA-K 0.000 claims description 4
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- 230000007613 environmental effect Effects 0.000 abstract 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 abstract description 2
- 230000003197 catalytic effect Effects 0.000 abstract description 2
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Abstract
本发明公开了一种同时脱除烟气中SO2和NOx的方法,属于环境保护与综合利用技术领域。本发明将水溶性钌盐与氨水混合均匀得到钌胺络合物水溶液;其中钌胺络合物水溶液中钌离子的浓度为0.03~0.20 mol/L,氨水中氮元素与水溶性钌盐中钌元素的摩尔比为(8~50):1;在温度为5~60℃、pH值为7.5~12条件下,将烟气与钌胺络合物水溶液逆流接触反应得到溶液A和净化气体;其中烟气中氧气体积含量为0.5%~10%,烟气与钌胺络合物水溶液的气液体积比为(0.05~8):1;将溶液A排入结晶池中结晶分离铵盐得到溶液B,溶液B返回取代钌胺络合物水溶液。本发明利用钌胺络合物与NO的强络合能力和烟气中的余氧,液相催化氧化NOx转化为硝酸铵,NOx和SO2的去除效率高。
Description
技术领域
本发明涉及一种同时脱除烟气中SO2和NOx的方法,属于环境保护与综合利用技术领域。
背景技术
目前市场使用最多的脱硫脱硝一体化技术不是严格意义上的同时脱硫脱硝技术,而是将成熟的脱硫技术与脱硝技术进行联合。如采用石灰石法脱硫和选择性催化(SCR)脱硝两种技术联用,即先对烟气进行脱硫,然后再进行脱硝。这种技术占地面积大、操作复杂、成本高、且存在二次污染等问题,这将限制了该技术的进一步推广应用。
目前一体化同时脱硫脱硝技术,包括活性炭(焦)法、石灰/尿素喷射法、臭氧法、H2O2法、氨法等,存在NOx选择性差,去除效率低,且投资高、运行费用能耗高、同时脱硫脱硝效果低,二次污染,因而无法达到工业化运行规模。电子束照射法、光催化法存在NOx除去不彻底,易产生NH3和N2O导致二次污染,且稳定性差、成本高以及硫硝不能回收利用。一体化脱硫脱硝技术在硫的去除方面效果较好,但由于NOx,特别是NO (超过90%,占NOx的比例)的水溶性差、低反应性活性,导致NO的脱除不理想。
发明内容
针对现有技术中一体化同时脱硫脱硝存在的问题,本发明提供一种同时脱除烟气中SO2和NOx的方法,本发明在钌胺络合物催化剂的催化作用下,利用烟气中的微量氧与NO反应,产生水溶性的NO2,再借助钌胺络合物水溶液的过量氨水去除NO2,同时产生硝酸铵;反应体系中的过量氨水与SO2充分反应,从而实现烟气的同步脱硫脱硝,并实现硫硝的资源化;反应的钌胺络合物可通过简单加热的方式再生,实现催化剂的循环利用,无二次污染问题。
一种同时脱除烟气中SO2和NOx的方法,具体步骤如下:
(1)将水溶性钌盐与氨水混合均匀得到钌胺络合物水溶液;其中钌胺络合物水溶液中钌离子的浓度为0.03~0.20 mol/L,氨水中氮元素与水溶性钌盐中钌元素的摩尔比为(8~50):1;
(2)在温度为5~60℃、pH值为7.5~12条件下,将烟气与步骤(1)钌胺络合物水溶液逆流接触反应得到溶液A和净化气体;其中烟气中氧气体积含量为0.5%~10%,烟气与钌胺络合物水溶液的气液体积比为(0.05~8):1;
(3)将步骤(2)溶液A排入结晶池中结晶分离铵盐得到溶液B,溶液B返回步骤(2)取代钌胺络合物水溶液;
所述水溶性钌盐为三氯化钌和/或碘化钌;
优选的,所述步骤(1)钌胺络合物水溶液中钌离子的浓度为0.08~0.15mol/L,氨水中氮元素与水溶性钌盐中钌元素的摩尔比为(20~50):1;
优选的,所述步骤(2)中温度为15~40℃,pH值为9~12;
优选的,所述步骤(2)中烟气与钌胺络合物水溶液的气液体积比为(0.05~5):1。
本发明的原理如下:
钌胺络合物与NO反应
[Ru(NH3)6]3+ + NO → [Ru(NH3)5(NO)]3+ + NH3 (1)
NO与烟气中余量氧反应(钌胺络合物再生)
[Ru(NH3)5(NO)]3+ + 1/2O2 + NH3 → [Ru(NH3)6]3+ + NO2 (2)
NO2与氨水反应
2NO2 + 2NH3·H2O + 1/2O2 → 2NH4NO3 + H2O (3)
SO2与氨水反应
SO2 + 2NH3·H2O + 1/2O2 → (NH4)2SO4 + H2O (4)
本发明的有益效果:
(1)本发明构建了同时脱硫脱硝的封闭循环系统,化学药剂种类和使用量少,工艺清洁环保;
(2)本发明利用钌胺络合物催化剂,可以同时脱硫脱硝,并且在反应过程中可自行再生,无需单独再生,提高了工艺系统的稳定性,降低投资和运行成本;
(3)本发明返回可同时脱硫脱硝,SO2和NOx的去除率可高达100%;
(4)本发明烟气中氮硫可实现资源化,避免传统技术对氮硫资源的抛弃,经济效益高。
附图说明
图1为钌胺络合物脱硫脱硝工艺示意图。
具体实施方式
下面结合具体实施方式对本发明作进一步详细说明,但本发明的保护范围并不限于所述内容。
实施例1:本实施例中待处理烟气铜冶炼烟气,含有SO2 2500 mg/m3、NOx 300 mg/m3、O2体积含量为0.5%;
如图1所示,一种同时脱除烟气中SO2和NOx的方法,具体步骤如下:
(1)将水溶性钌盐(碘化钌)与氨水混合均匀得到钌胺络合物水溶液;其中钌胺络合物水溶液中钌离子的浓度为0.03 mol/L,氨水中氮元素与水溶性钌盐中钌元素的摩尔比为8:1;
(2)在温度为5℃、pH值为8.0条件下,将烟气与步骤(1)钌胺络合物水溶液通入反应装置中逆流接触反应得到溶液A和净化气体;其中烟气中氧气体积含量为0.5%,烟气与钌胺络合物水溶液的气液体积比为0.05:1;
(3)将步骤(2)溶液A排入结晶池中结晶分离铵盐得到溶液B,溶液B返回步骤(2)取代钌胺络合物水溶液;
通过工业质谱仪分析气体出口中SO2的排放浓度为25 mg/m3,NOx的排放浓度为5mg/m3。
实施例2:本实施例中待处理烟气铜冶炼烟气,含有SO2 3000 mg/m3、NOx 250 mg/m3、O2体积含量为2%;
如图1所示,一种同时脱除烟气中SO2和NOx的方法,具体步骤如下:
(1)将水溶性钌盐(碘化钌和三氯化钌)与氨水混合均匀得到钌胺络合物水溶液;其中钌胺络合物水溶液中钌离子的浓度为0.08 mol/L,氨水中氮元素与水溶性钌盐中钌元素的摩尔比为15:1;
(2)在温度为20℃、pH值为9.0条件下,将烟气与步骤(1)钌胺络合物水溶液通入反应装置中逆流接触反应得到溶液A和净化气体;其中烟气中氧气体积含量为2%,烟气与钌胺络合物水溶液的气液体积比为2:1;
(3)将步骤(2)溶液A排入结晶池中结晶分离铵盐得到溶液B,溶液B返回步骤(2)取代钌胺络合物水溶液;
通过工业质谱仪分析气体出口中SO2的排放浓度为5 mg/m3,NOx的排放浓度为1.8mg/m3。
实施例3:本实施例中待处理烟气铜冶炼烟气,含有SO2 2800 mg/m3、NOx 270 mg/m3、O2体积含量为5%;
如图1所示,一种同时脱除烟气中SO2和NOx的方法,具体步骤如下:
(1)将水溶性钌盐(三氯化钌)与氨水混合均匀得到钌胺络合物水溶液;其中钌胺络合物水溶液中钌离子的浓度为0.15mol/L,氨水中氮元素与水溶性钌盐中钌元素的摩尔比为40:1;
(2)在温度为40℃、pH值为10.0条件下,将烟气与步骤(1)钌胺络合物水溶液通入反应装置中逆流接触反应得到溶液A和净化气体;其中烟气中氧气体积含量为5%,烟气与钌胺络合物水溶液的气液体积比为5:1;
(3)将步骤(2)溶液A排入结晶池中结晶分离铵盐得到溶液B,溶液B返回步骤(2)取代钌胺络合物水溶液;
通过工业质谱仪分析气体出口中SO2的排放浓度为19mg/m3,NOx的排放浓度为3.2mg/m3。
实施例4:本实施例中待处理烟气铜冶炼烟气,含有SO2 3500 mg/m3、NOx 330 mg/m3、O2体积含量为10%;
如图1所示,一种同时脱除烟气中SO2和NOx的方法,具体步骤如下:
(1)将水溶性钌盐(三氯化钌)与氨水混合均匀得到钌胺络合物水溶液;其中钌胺络合物水溶液中钌离子的浓度为0.2mol/L,氨水中氮元素与水溶性钌盐中钌元素的摩尔比为60:1;
(2)在温度为60℃、pH值为12.0条件下,将烟气与步骤(1)钌胺络合物水溶液通入反应装置中逆流接触反应得到溶液A和净化气体;其中烟气中氧气体积含量为10%,烟气与钌胺络合物水溶液的气液体积比为8:1;
(3)将步骤(2)溶液A排入结晶池中结晶分离铵盐得到溶液B,溶液B返回步骤(2)取代钌胺络合物水溶液;
通过工业质谱仪分析气体出口中SO2的排放浓度为22mg/m3,NOx的排放浓度为4.3mg/m3。
对比例:待处理烟气铜冶炼烟气,含有SO2 2800 mg/m3、NOx 270 mg/m3、O2体积含量为5%;
以铜冶炼烟气为处理气体,氨水打入反应装置中,氨水与铜冶炼烟气中的SO2和NOx逆向接触充分反应,并控制烟气与氨水溶液的气液比为5,反应温度为40℃,反应pH值为10;通过工业质谱仪分析气体出口中SO2和NOx的排放浓度分别为80 mg/m3和212 mg/m3。
Claims (5)
1.一种同时脱除烟气中SO2和NOx的方法,其特征在于,具体步骤如下:
(1)将水溶性钌盐与氨水混合均匀得到钌胺络合物水溶液;其中钌胺络合物水溶液中钌离子的浓度为0.03~0.20 mol/L,氨水中氮元素与水溶性钌盐中钌元素的摩尔比为(8~50):1;
(2)在温度为5~60℃、pH值为7.5~12条件下,将烟气与步骤(1)钌胺络合物水溶液逆流接触反应得到溶液A和净化气体;其中烟气中氧气体积含量为0.5%~10%,烟气与钌胺络合物水溶液的气液体积比为(0.05~8):1;
(3)将步骤(2)溶液A排入结晶池中结晶分离铵盐得到溶液B,溶液B返回步骤(2)取代钌胺络合物水溶液。
2.根据权利要求1所述同时脱除烟气中SO2和NOx的方法,其特征在于:水溶性的钌盐为三氯化钌和/或碘化钌。
3.根据权利要求1所述利用磷石膏和热闷钢渣制备合成气的方法,其特征在于:步骤(1)钌胺络合物水溶液中钌离子的浓度为0.08~0.15mol/L,氨水中氮元素与水溶性钌盐中钌元素的摩尔比为(20~50):1。
4.根据权利要求1所述利用磷石膏和热闷钢渣制备合成气的方法,其特征在于:步骤(2)中温度为15~40℃,pH值为9~12。
5.根据权利要求1所述利用磷石膏和热闷钢渣制备合成气的方法,其特征在于:步骤(2)中烟气与钌胺络合物水溶液的气液体积比为(0.05~5):1。
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