CN101600499A - 废气处理催化剂和废气处理系统 - Google Patents
废气处理催化剂和废气处理系统 Download PDFInfo
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- 239000003054 catalyst Substances 0.000 title claims abstract description 128
- 239000002912 waste gas Substances 0.000 title claims abstract description 40
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims abstract description 54
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 45
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims abstract description 42
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims abstract description 36
- 239000000463 material Substances 0.000 claims abstract description 30
- 239000011248 coating agent Substances 0.000 claims abstract description 29
- 238000000576 coating method Methods 0.000 claims abstract description 29
- 229910021529 ammonia Inorganic materials 0.000 claims abstract description 27
- 239000004408 titanium dioxide Substances 0.000 claims abstract description 21
- 229910052697 platinum Inorganic materials 0.000 claims abstract description 19
- 239000003638 chemical reducing agent Substances 0.000 claims abstract description 9
- 150000001875 compounds Chemical class 0.000 claims abstract description 7
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims abstract description 7
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229910052750 molybdenum Inorganic materials 0.000 claims abstract description 6
- 239000011733 molybdenum Substances 0.000 claims abstract description 6
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229910052721 tungsten Inorganic materials 0.000 claims abstract description 6
- 239000010937 tungsten Substances 0.000 claims abstract description 6
- 239000002002 slurry Substances 0.000 claims description 9
- 238000011144 upstream manufacturing Methods 0.000 claims description 3
- 239000000758 substrate Substances 0.000 abstract description 10
- 230000003197 catalytic effect Effects 0.000 abstract description 2
- 239000003517 fume Substances 0.000 abstract 1
- 239000000203 mixture Substances 0.000 description 12
- 238000002156 mixing Methods 0.000 description 11
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Chemical compound [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 description 10
- 239000010410 layer Substances 0.000 description 10
- 238000006243 chemical reaction Methods 0.000 description 6
- 238000001035 drying Methods 0.000 description 6
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 6
- 239000007864 aqueous solution Substances 0.000 description 5
- 230000001588 bifunctional effect Effects 0.000 description 5
- 238000000034 method Methods 0.000 description 5
- 238000001354 calcination Methods 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- QGLKJKCYBOYXKC-UHFFFAOYSA-N nonaoxidotritungsten Chemical compound O=[W]1(=O)O[W](=O)(=O)O[W](=O)(=O)O1 QGLKJKCYBOYXKC-UHFFFAOYSA-N 0.000 description 4
- 239000010936 titanium Substances 0.000 description 4
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 4
- 229910001930 tungsten oxide Inorganic materials 0.000 description 4
- CLSUSRZJUQMOHH-UHFFFAOYSA-L platinum dichloride Chemical compound Cl[Pt]Cl CLSUSRZJUQMOHH-UHFFFAOYSA-L 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 235000011114 ammonium hydroxide Nutrition 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- XAYGUHUYDMLJJV-UHFFFAOYSA-Z decaazanium;dioxido(dioxo)tungsten;hydron;trioxotungsten Chemical compound [H+].[H+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.[O-][W]([O-])(=O)=O.[O-][W]([O-])(=O)=O.[O-][W]([O-])(=O)=O.[O-][W]([O-])(=O)=O.[O-][W]([O-])(=O)=O.[O-][W]([O-])(=O)=O XAYGUHUYDMLJJV-UHFFFAOYSA-Z 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 1
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- UNTBPXHCXVWYOI-UHFFFAOYSA-O azanium;oxido(dioxo)vanadium Chemical compound [NH4+].[O-][V](=O)=O UNTBPXHCXVWYOI-UHFFFAOYSA-O 0.000 description 1
- 238000000498 ball milling Methods 0.000 description 1
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- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
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- 239000011247 coating layer Substances 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
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- 229910000476 molybdenum oxide Inorganic materials 0.000 description 1
- 238000006864 oxidative decomposition reaction Methods 0.000 description 1
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical compound [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 description 1
- PIBWKRNGBLPSSY-UHFFFAOYSA-L palladium(II) chloride Chemical compound Cl[Pd]Cl PIBWKRNGBLPSSY-UHFFFAOYSA-L 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000007493 shaping process Methods 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- ZNOKGRXACCSDPY-UHFFFAOYSA-N tungsten trioxide Chemical compound O=[W](=O)=O ZNOKGRXACCSDPY-UHFFFAOYSA-N 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
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Abstract
本发明提供一种能够降低氨泄漏率同时保持足够的NOx除去效率的废气处理催化剂，所述催化剂包含涂层和催化剂基材，其中所述涂层相对于催化剂基材具有降低的厚度；并涉及使用所述废气处理催化剂的废气处理系统。用于通过使用氨作为还原剂从废气催化地除去氮氧化物同时分解和除去未反应氨的该废气处理催化剂中，在多孔催化剂基材的表面上形成涂层，所述涂层包括负载于二氧化钛上的铂，该多孔催化剂基材包含二氧化钛和选自钒(V)的氧化物、钨(W)的氧化物和钼(Mo)的氧化物的至少一种化合物。
Description
技术领域
本发明涉及废气处理催化剂和废气处理系统。
背景技术
为了使燃烧废气脱硝，氨(NH3)被用作用于将氮氧化物(NOx)分解为氮气(N2)和水蒸气(H2O)的还原剂。在这种脱硝反应中，为了提高反应速率和反应效率，使用DeNOx(脱硝)催化剂。为了提高NOx的分解率，当添加NH3时仅仅需要提高NH3/NOx摩尔比。然而，当NH3/NOx摩尔比过度增加时，未反应的氨可能混入废气中。当将所得到的废气释放到大气中时，由于泄漏的氨，可能引起二次污染等等。
在这种状况下，JP3436567 B中公开了具有用于氧化未反应氨的催化剂层的废气净化催化剂。
这种废气净化催化剂包含使用DeNOx催化剂浆料形成的厚约0.5mm的DeNOx催化剂层。该层对于确保脱硝反应是必不可少的。然而，DeNOx催化剂层的加厚增加了压力损失，使得工厂的工作效率退化。加厚DeNOx催化剂层的另一个原因是催化剂载体层不能用作废气净化催化剂。
发明内容
本发明要解决的问题
鉴于以上状况而作出了本发明。本发明的目的是提供一种废气处理催化剂和一种废气处理系统，其能够降低氨泄漏率同时保持足够的NOx除去效率，包含催化剂基材和涂层，其中所述涂层相对于该催化剂基材具有降低的厚度。
解决问题的手段
为了实现以上目的，本发明的特征可在于能够在使用氨作为还原剂从废气中催化地除去氮氧化物的同时分解和除去未反应的氨的废气处理催化剂，该催化剂包含：包含二氧化钛及选自钒(V)的氧化物、钨(W)的氧化物和钼(Mo)的氧化物的至少一种化合物的多孔催化剂基材；以及在该多孔催化剂基材的表面上形成的涂层，所述涂层包含负载在二氧化钛上的铂。
在一个方面，本发明可以是通过使用氨作为还原剂能够从废气中催化地除去氮氧化物同时分解和除去未反应的氨的废气处理催化剂，其通过如下操作获得：将包含负载在二氧化钛上的铂的第一催化剂浆料与由二氧化钛及选自钒(V)的氧化物、钨(W)的氧化物和钼(Mo)的氧化物的至少一种化合物制备的第二催化剂浆料混合，以形成浆料混合物；以及将该浆料混合物应用于该多孔催化剂基材的表面。
基于涂层中包含的二氧化钛和铂(Pt)的总量，优选该涂层可以包含0.05～0.1重量％的量的铂。
在本发明的废气处理催化剂中，该涂层的厚度可以优选为100～300μm。
在本发明的废气处理催化剂的一个实施方式中，该涂层中的铂可以与钒的氧化物不邻接。
在另一个方面，本发明的特征可在于能够在使用氨作为还原剂从废气中催化地除去氮氧化物的同时分解和除去未反应的氨的废气处理系统，其中DeNOx催化剂位于气流上游侧，本发明的废气处理催化剂布置在该DeNOx催化剂下游。
发明效果
本发明提供废气处理催化剂和废气处理系统，其相对于催化剂基材的厚度具有厚度减少的涂层，并具有降低的氨泄漏率同时保持足够的NOx除去效率。
具体实施方式
下文将参照实施方式更具体地描述本发明的废气处理催化剂和废气处理系统。
多孔催化剂基材
本发明的废气处理催化剂使用多孔催化剂基材作为基材。该多孔催化剂基材优选为多孔蜂窝催化剂基材。
具体地，使用二氧化钛和选自钒(V)的氧化物、钨(W)的氧化物和钼(Mo)的氧化物的至少一种化合物作为原材料形成该多孔催化剂基材。
通常，优选以(0.1～0.6)/(3～9)/(70～80)的V/W/Ti原子比或者(0.1～0.6)/(3～9)/(70～80)的V/Mo/Ti原子比混合原材料。
含有DeNOx催化剂成分的基材例如通过下列步骤制备：将氨水添加至偏钛酸浆料；添加预定量的仲钨酸铵粉末；混炼所得到的混合物；干燥并煅烧混炼的物质(mass)以获得催化剂粉末；将所得到的催化剂粉末和如果必要的成形助剂放入混炼机中；将所得到的混合物与足够量的水一起混炼；挤出所得到的物质；以及干燥然后煅烧该挤出物。由此制备的基材优选调节为具有0.25～0.40g/cc的孔隙体积。
该多孔催化剂基材充当用于分解源自废气的氮氧化物(NOx)和在分解氨过程中产生的氮氧化物两者的DeNOx催化剂。
在本发明的废气处理催化剂中，该多孔催化剂基材充当DeNOx催化剂。因为它分解未反应的氨，同时分解在分解氨过程中产生的氮氧化物(NOx)，所以它不会导致脱硝效率的恶化。
含有在其上负载铂的二氧化钛的涂层
在本发明的废气处理催化剂中，在如上制备的多孔催化剂基材上形成涂层。该涂层含有在其上负载铂的二氧化钛。
该涂层可形成为单层的形式，作为氨氧化催化剂和DeNOx催化剂，该单层包含在其上负载铂的二氧化钛。
具有涂层的废气处理催化剂的制备方法
通过制备催化剂浆料，将它施用于多孔催化剂基材，以及煅烧所得到的材料，从而制备涂层。下面是这种方法的一个实例。
在这种方法的一个实施方式中，将球形二氧化钛(具有2～4mm的直径)浸渍在诸如氯化铂水溶液(H2PtCl6)的水性铂溶液中，从而在该球形二氧化钛上负载0.05～0.1重量％的Pt。干燥之后，将所得到的二氧化钛在450～500℃煅烧3～5小时以获得粉末催化剂1。将水加入所得到的粉状催化剂1，接着进行湿式球磨粉碎以获得催化剂浆料1(氨氧化催化剂浆料)。
类似地，通过混合选自钒氧化物、钨氧化物和钼氧化物的至少一种化合物和二氧化钛而获得粉末催化剂2，向其中加入水，以及在湿式球磨机中粉碎所得到的混合物，以获得催化剂浆料(DeNOx催化剂浆料)2。在这种情况下，优选以(0.1～0.6)/(3～9)/(70～80)的V/W/Ti原子比或者(0.1～0.6)/(3～9)/(70～80)的V/Mo/Ti原子比混合该氧化物。
通过混合30～40重量份的催化剂浆料1和60～70重量份的催化剂浆料2，制备催化剂浆料3，所述催化剂浆料1和2分别调节为相等的浆料浓度。
将多孔催化剂基材，例如多孔蜂窝催化剂基材浸渍入催化剂浆料3。干燥所得到的催化剂之后，将它在450～500℃煅烧3～5小时。以该基材表面积每平方米85～115g(该涂层的厚度为85～115μm)的量，将催化剂浆料3施用于该基材的表面。由此获得的双功能催化剂是在其多孔催化剂基材上具有涂层的废气处理催化剂，即氨氧化催化剂和DeNOx催化剂，该涂层由含有在其上负载铂的二氧化钛的单层构成。
当该涂层由如上所述的单层制成时，为了提高铂在氨氧化时的催化活性，优选使钒氧化物与铂不邻接。
本发明的废气处理催化剂用作通过使用氨作为还原剂从废气中催化地除去氮氧化物，同时所述催化剂还分解和除去未反应的氨。简而言之，它经历如下所述的脱硝反应和氨的氧化分解。
脱硝反应
NO+NH3+1/4O2＝N2+3/2H2O (1)
氨的氧化分解反应
NH3+3/4O2＝1/2N2+3/2H2O (2)
NH3+5/4O2＝NO+3/2H2O (3)
本发明的废气处理催化剂能够用于废气处理系统。这种废气处理系统是通过使用氨作为还原剂从废气中催化地除去氮氧化物，并且同时分解和除去未反应的氨的废气处理系统。作为具体方式，废气处理系统能够通过如下操作构建：将DeNOx催化剂布置在气流上游侧，然后将本发明的废气处理催化剂布置在该DeNOx催化剂下游。
与仅使用DeNOx催化剂的系统相比较，这种废气处理系统具有NH3的泄漏量降低的优点。
实施例1：
将球形二氧化钛(具有2～4mm的直径)浸渍在氯化铂水溶液(H2PtCl6)中，从而在球形二氧化钛上负载0.05重量％的铂。在干燥之后，将所得到的二氧化钛在500℃煅烧5小时以获得粉末催化剂1。将水加入所得到的粉末催化剂(氨氧化催化剂)1，接着在湿式球磨机中粉碎以获得催化剂浆料1。类似地，将水加入由0.6重量份的钒氧化物、9重量份的钨氧化物和80重量份的二氧化钛构成的粉末催化剂(DeNOx催化剂)2中，并且在球磨机中粉碎所得到的混合物以获得催化剂浆料2。
催化剂浆料3通过混合35重量份的催化剂浆料1和65重量份的催化剂浆料2而制备，所述催化剂浆料1和2均调节为相等的浆料浓度。将用作多孔催化剂基材且由0.6重量份的钒氧化物、9重量份的钨氧化物和80重量份的二氧化钛构成的多孔蜂窝催化剂基材(起DeNOx催化剂的作用)浸渍在催化剂浆料3中。干燥所得到的催化剂，然后在500℃煅烧5小时。
以该基材表面积每平方米100g(涂层厚度：约100μm)的量将催化剂浆料3施用于该基材，所得到的蜂窝废气处理催化剂指定为双功能催化剂1。
实施例2
按用于实施例1的双功能催化剂1类似的方式获得双功能催化剂2，所不同的是，铂(Pt)的负载量变为0.1重量％。
比较例1
以下面的方式制备TiO2-V2O5-WO3DeNOx催化剂(TiO2∶V2O5∶WO3质量比＝80∶0.6∶9)。
将具有25％NH3含量的氨水添加至3600g的偏钛酸浆料(具有30质量％的TiO2含量)，以将pH调节至6.5。将仲钨酸铵粉末添加至所得到的混合物中从而得到9质量％的WO3含量，并将所得到的混合物湿法混炼2小时。将所得到的物质干燥，然后在550℃煅烧5小时以获得由二氧化钛和钨氧化物构成的粉末。将偏钒酸铵水溶液添加至所得到的粉末中，从而得到0.6质量％的V2O5含量。将所得到的混合物充分混合、干燥并在450℃煅烧4小时，以获得由二氧化钛[TiO2]、钒氧化物[V2O5]和钨氧化物[WO3]构成的粉末(A)。将1000g粉末(A)、25g羧甲基纤维素和12.5g聚环氧乙烷填充入混炼机。向所得到的混合物加入足够量的水，接着混炼30分钟。将所得到的混炼物质挤出成50mm2的片材，将该片材干燥然后在500℃煅烧5小时。
比较例2
按用于实施例1的类似方式制备催化剂，所不同的是，使用氯化钯水溶液代替氯化铂水溶液(H2PtCl6)。
使用双功能催化剂1、2和5以及DeNOx催化剂进行性能试验。
在下列条件下进行性能试验。
废气温度：380℃
废气流速：2.3Nm/秒
NOx浓度：500ppm
结果示于表1。
表1
使用本发明的废气处理催化剂能够降低泄漏的氨浓度，同时保持95％的脱硝效率，还能够降低涂层的厚度。
Claims (5)
1.一种废气处理催化剂，其能够在使用氨作为还原剂从废气中催化地除去氮氧化物的同时分解和除去未反应的氨，该催化剂包含：
多孔催化剂基材，其包含二氧化钛及选自钒(V)的氧化物、钨(W)的氧化物和钼(Mo)的氧化物的至少一种化合物；以及
在该多孔催化剂基材的表面上形成的涂层，所述涂层包含负载于二氧化钛上的铂。
2.根据权利要求1的废气处理催化剂，其通过如下获得：将包含负载于二氧化钛上的铂的第一催化剂浆料与由二氧化钛及选自钒(V)的氧化物、钨(W)的氧化物和钼(Mo)的氧化物的至少一种化合物制备的第二催化剂浆料混合，从而形成浆料混合物；以及将该浆料混合物应用于该多孔催化剂基材的表面。
3.根据权利要求1或2的废气处理催化剂，其中基于该涂层中包含的二氧化钛和铂(Pt)的总量，该涂层包含0.05～0.1重量％的量的铂。
4.根据权利要求1的废气处理催化剂，其中该涂层具有100～300μm的厚度。
5.一种废气处理系统，其能够在使用氨作为还原剂从废气中催化地除去氮氧化物的同时分解和除去未反应的氨，其中DeNOx催化剂布置在气流上游，且如权利要求1～4中任一项所述的废气处理催化剂布置在该DeNOx催化剂下游。
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| JP3219613B2 (ja) | 1994-11-14 | 2001-10-15 | 三菱重工業株式会社 | アンモニア分解触媒及びアンモニアの分解除去方法 |
| JPH08252459A (ja) * | 1995-01-17 | 1996-10-01 | Toyota Central Res & Dev Lab Inc | 酸化触媒 |
| JP3389005B2 (ja) | 1996-06-25 | 2003-03-24 | 三菱重工業株式会社 | 窒素酸化物除去触媒 |
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| US7393511B2 (en) * | 2005-02-16 | 2008-07-01 | Basf Catalysts Llc | Ammonia oxidation catalyst for the coal fired utilities |
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2007
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| CN104812486A (zh) * | 2012-11-30 | 2015-07-29 | 庄信万丰股份有限公司 | 氨氧化催化剂 |
| CN104812486B (zh) * | 2012-11-30 | 2019-02-12 | 庄信万丰股份有限公司 | 氨氧化催化剂 |
| CN107427826A (zh) * | 2015-03-27 | 2017-12-01 | 丰田自动车株式会社 | 废气净化用催化剂 |
| CN107427826B (zh) * | 2015-03-27 | 2021-01-12 | 丰田自动车株式会社 | 废气净化用催化剂 |
| CN105221489A (zh) * | 2015-11-14 | 2016-01-06 | 无锡清杨机械制造有限公司 | 一种带净化功能的卫浴抽风机 |
| CN110494205A (zh) * | 2017-03-30 | 2019-11-22 | 庄信万丰股份有限公司 | 用于排放处理系统中的具有scr活性基材、氨泄漏催化剂层和scr层的催化剂制品 |
| CN110494205B (zh) * | 2017-03-30 | 2022-10-14 | 庄信万丰股份有限公司 | 用于排放处理系统中的具有scr活性基材、氨泄漏催化剂层和scr层的催化剂制品 |
| CN112536061A (zh) * | 2019-09-23 | 2021-03-23 | 中国石油化工股份有限公司 | 一种废气处理催化剂及其制备方法 |
| CN112536061B (zh) * | 2019-09-23 | 2023-05-02 | 中国石油化工股份有限公司 | 一种废气处理催化剂及其制备方法 |
Also Published As
| Publication number | Publication date |
|---|---|
| CN101600499B (zh) | 2013-02-13 |
| BRPI0807419B1 (pt) | 2017-06-13 |
| EP2179792B1 (en) | 2016-06-08 |
| CA2677060C (en) | 2013-12-24 |
| KR20090101237A (ko) | 2009-09-24 |
| WO2009025185A1 (ja) | 2009-02-26 |
| JP5192754B2 (ja) | 2013-05-08 |
| CA2677060A1 (en) | 2009-02-26 |
| EP2179792A4 (en) | 2011-08-03 |
| KR101087374B1 (ko) | 2011-11-25 |
| RU2406567C1 (ru) | 2010-12-20 |
| US8202481B2 (en) | 2012-06-19 |
| EP2179792A1 (en) | 2010-04-28 |
| US20100080737A1 (en) | 2010-04-01 |
| BRPI0807419A2 (pt) | 2014-05-27 |
| JP2009045586A (ja) | 2009-03-05 |
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