CN108025291B - 用于去除烟气和废气中氮氧化物的蜂窝状催化剂及其制备方法 - Google Patents
用于去除烟气和废气中氮氧化物的蜂窝状催化剂及其制备方法 Download PDFInfo
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- 239000003546 flue gas Substances 0.000 title description 8
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title description 5
- 238000002360 preparation method Methods 0.000 title description 2
- 239000002912 waste gas Substances 0.000 title description 2
- 239000010410 layer Substances 0.000 claims abstract description 25
- 239000012792 core layer Substances 0.000 claims abstract description 22
- 239000000203 mixture Substances 0.000 claims abstract description 14
- GNTDGMZSJNCJKK-UHFFFAOYSA-N divanadium pentaoxide Chemical group O=[V](=O)O[V](=O)=O GNTDGMZSJNCJKK-UHFFFAOYSA-N 0.000 claims description 14
- 238000000034 method Methods 0.000 claims description 13
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 12
- 239000000758 substrate Substances 0.000 claims description 11
- 229910052720 vanadium Inorganic materials 0.000 claims description 10
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims description 10
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Abstract
本发明公开了一种钒氧化物基蜂窝状SCR催化剂,所述钒氧化物基蜂窝状SCR催化剂由多个波纹片材构成,所述多个波纹片材彼此层叠以形成多个流通通道,所述波纹片材设置有惰性内芯层和含有SCR催化剂组合物的最外层。
Description
本发明涉及去除固定烟气源(包括燃气轮机和发电厂)产生的废气和烟气中的氮氧化物即NOx。
本发明特别涉及一种蜂窝形的选择性催化还原(SCR)催化剂,其用于去除化石燃料(如天然气、煤或石油)燃烧时在固定污染源中形成的烟气中的氮氧化物。
利用SCR方法从固定污染源去除氮氧化物的方法在本领域是公知的。
在SCR方法中,可以通过在存在催化剂的情况下,利用还原剂(通常为氨)将烟气中的NOx含量转化为游离氮,来将NOx含量去除或基本上减少,所述转化如下列反应所示:
4NO+4NH3+O2-4N2+6H2O
NO+NO2+2NH3-2N2+3H2O
用于净化固定污染源产生的烟气的最典型SCR催化剂组合物是基于钒氧化物的。
在存在暴露于高硫燃料的风险的情况下,为了避免高硫酸盐排放,钒基SCR催化剂是特别优选的。钒基SCR催化剂的优点是这些催化剂具有相对较低的硫氧化活性,这在用于净化含硫氧化物的烟气时特别重要。
钒基SCR催化剂的催化活性组分由支承在二氧化钛上的五氧化二钒和三氧化钨组成。为了净化固定污染源产生的气体,将催化剂洗涂在整体料基板上,该基板典型地由层叠起来的陶瓷材料波纹片材或非织造玻璃纤维组成,这些材料形成具有多个平行的流通通道的蜂窝结构。
即使具有低的硫氧化活性,钒基催化剂实际上也会使SO2氧化成SO3。SO3可以与NH3反应形成硫酸氢铵,这可能会导致催化剂和下游设备发生结垢和堵塞。
熟知的是,在典型的SCR反应条件下,SCR反应比NO和NH3扩散进入催化剂壁快得多。NO的去除主要取决于整体料的比表面积。这意味着减小整体料的壁厚在很大程度上不会对该整体料的活性造成负面影响。从理论上讲,从活性的角度来看,壁厚仅为市售SCR整体料的20%的SCR催化剂在典型的高粉尘条件下具有相同的活性。然而,这样的催化剂会遭受腐蚀和机械不稳定性。
另一方面,SO2氧化反应比SO2在催化剂壁中的扩散要慢得多。这意味着整个催化剂壁有助于SO2氧化成SO3。当氧化钒是这种不希望的反应的活性位点时,通常减少催化剂上装载的氧化钒的量以尽量减少不希望的还原。然而,这也具有将SCR反应速率降低至较小程度的效果。
减少SO2到SO3转化的另一种更有效的方法可以是减小催化剂壁的厚度。但是,当减小壁厚时,经过减小的壁厚必须仍然保持蜂窝结构有足够的稳定性。当为基板的壁提供惰性粘土材料的内芯层时,本发明解决了该问题。
因此,本发明提供了一种蜂窝状SCR催化剂,该蜂窝状SCR催化剂由多个波纹片材构成,该多个波纹片材彼此层叠以形成多个流通通道,
每个波纹片材包括内芯层和最外层,所述内芯层包括缠结非织造纤维,该非织造纤维在每个波纹片材的两个侧面上涂覆有粘土材料,所述最外层支承在内芯层的两个侧面上,所述最外层包含SCR催化剂组合物,所述内芯层构成通道壁介于50%和95%之间的厚度。
根据本发明的催化剂具有如下优点,即由于内部粘土芯层而保留了整体料壁的总体厚度,所以它显示出至少与常规整体料一样良好的结构稳定性。
本发明降低了每单位体积的整体料的催化剂负载,导致减少了SO2氧化。同时,所减少的催化剂绝对量允许增加外层中的氧化钒含量,从而使催化最外层的NO还原活性最大化。
另一个优点是内芯上的外层为催化剂结构提供机械稳定性,并同时减少SO2氧化。外层防止表面出现额外的干裂。这也可以改善结构的耐冲蚀磨损性和机械稳定性,因为去除了颗粒在高冲击角度下冲击该结构所在的磨损点。
根据本发明的催化剂的具体特征是上述单独的优点或其组合,其中
非织造纤维为玻璃纤维;
内芯层还包含硅藻土,
内芯层具有介于0.6mm和1.2mm之间的层厚度;
最外层具有介于0.05mm和0.6mm之间的层厚度;
SCR催化剂组合物包含二氧化钛和五氧化二钒;
SCR催化剂组合物包含二氧化钛、五氧化二钒和钨的氧化物;
最外层中五氧化二钒的量介于1重量%至5重量%之间;
SCR催化剂还包括布置在每个波纹片材上的衬垫。
本发明的另一方面是一种制备具有多个流通通道的蜂窝状SCR催化剂的方法,该方法包括以下步骤:
(a)提供缠结非织造纤维片材;
(b)将片材加工成波纹;
(c)将在步骤(b)中获得的波纹片材层叠以形成蜂窝结构化基板;
(d)用粘土材料涂覆该蜂窝结构化基板的波纹片材以获得每个波纹片材的内芯层,并且干燥和/或煅烧该蜂窝结构化基板;
(e)用包含SCR催化剂组合物或其前体的催化剂涂层涂覆该蜂窝结构化基板中的每个波纹片材的内芯层的每个侧面;以及
(f)煅烧步骤(e)的已涂覆的蜂窝结构化基板以获得蜂窝状SCR催化剂。
根据本发明的方法的具体特征是上述单独的步骤或其组合,其中
在步骤(b)中获得的每个波纹片材在层叠之前衬有衬垫;
非织造纤维为玻璃纤维;
内芯材料还包括硅藻土;
催化剂涂层具有介于0.05mm和0.3mm之间的层厚度;
内芯层具有介于O.6mm和1.2mm之间的层厚度;
SCR催化剂组合物包含二氧化钛和钒的氧化物;
钒的氧化物为在最外层中以介于1重量%至5重量%的量施用的五氧化二钒;并且
SCR催化剂组合物还包含钨的氧化物;
在所有的特征和方面中,粘土材料可以选自高岭土族、含水硅酸铝、绿泥石族、叶腊石族、膨润土或其混合物。
实施例
图1示出了根据本发明的蜂窝状SCR催化剂与已知的蜂窝状SCR催化剂的DeNOx活性与SO2氧化活性的比率对比,其中本发明的蜂窝状SCR催化剂具有厚度为0.7mm的内芯层和在芯层每个侧面上厚度为0.15mm的催化剂外层,而已知的蜂窝状SCR催化剂具有支承在波纹玻璃纤维纸上的全催化剂层。这两个比率已根据全催化剂层的值来归一化。理想的是具有尽可能高的DeNOx活性与SO2氧化活性比率。
从图1可以明显看出,根据本发明的惰性内芯催化剂在DeNOx:SO2氧化活性方面比全催化剂层高/好约58%。
Claims (14)
1.一种蜂窝状SCR催化剂,所述蜂窝状SCR催化剂由多个波纹片材构成,所述多个波纹片材彼此层叠以形成多个流通通道,
每个缠结非织造纤维的波纹片材在波纹片材的两个侧面上涂覆有粘土材料的内芯层,其中所述内芯层具有介于0.6mm和1.2mm之间的层厚度,和支承在所述内芯层的两个侧面上的最外层,所述最外层包含SCR催化剂组合物,其中所述最外层具有介于0.05mm和0.6mm之间的层厚度,并且其中所述SCR催化剂组合物包含二氧化钛和钒的氧化物,和所述内芯层构成通道壁介于50%和95%之间的厚度。
2.根据权利要求1所述的蜂窝状SCR催化剂,其中所述非织造纤维为玻璃纤维。
3.根据权利要求1或2所述的蜂窝状SCR催化剂,其中内芯层还包含硅藻土。
4.根据权利要求1所述的蜂窝状SCR催化剂,其中所述钒的氧化物为含量介于1重量%和5重量%之间的五氧化二钒。
5.根据权利要求1所述的蜂窝状SCR催化剂,还包含钨的氧化物。
6.根据权利要求1所述的蜂窝状SCR催化剂,还包括布置在每个所述波纹片材上的衬垫。
7.根据权利要求1所述的蜂窝状SCR催化剂,其中所述内芯层还包含硅藻土。
8.一种制备具有多个流通通道的蜂窝状SCR催化剂的方法,所述方法包括以下步骤:
(a)提供缠结非织造纤维片材;
(b)将所述片材加工成波纹;
(c)将在步骤(b)中获得的波纹片材层叠以形成蜂窝结构化基板;
(d)用粘土材料涂覆所述蜂窝结构化基板的所述波纹片材以获得每个所述波纹片材的内芯层,其中所述内芯层具有介于0.6mm和1.2mm之间的层厚度,并且干燥和/或煅烧所述蜂窝结构化基板;
(e)用包含SCR催化剂组合物或其前体的催化剂涂层涂覆所述蜂窝结构化基板中的每个所述波纹片材的所述内芯层的每个侧面,其中所述SCR催化剂组合物包含二氧化钛和钒的氧化物,并且其中所述催化剂涂层具有介于0.05mm和0.6mm之间的层厚度;以及
(f)煅烧步骤(e)的所述蜂窝结构化基板以获得所述蜂窝状SCR催化剂。
9.根据权利要求8所述的方法,其中在步骤(b)中获得的每个波纹片材在层叠之前衬有衬垫。
10.根据权利要求9所述的方法,其中所述衬垫涂覆有粘土材料。
11.根据权利要求8所述的方法,其中所述非织造纤维为玻璃纤维。
12.根据权利要求8所述的方法,其中所述粘土材料还包括硅藻土。
13.根据权利要求8所述的方法,其中所述钒的氧化物为以介于1重量%至5重量%的量施用的五氧化二钒。
14.根据权利要求8所述的方法,其中所述SCR催化剂组合物还包含钨的氧化物。
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CN108025291A (zh) | 2018-05-11 |
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