CN103079691A - 提高耐用性的用于选择性催化还原的催化剂 - Google Patents

提高耐用性的用于选择性催化还原的催化剂 Download PDF

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CN103079691A
CN103079691A CN2011800420017A CN201180042001A CN103079691A CN 103079691 A CN103079691 A CN 103079691A CN 2011800420017 A CN2011800420017 A CN 2011800420017A CN 201180042001 A CN201180042001 A CN 201180042001A CN 103079691 A CN103079691 A CN 103079691A
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韩贤植
金振远
金垠锡
韩在煜
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Xi Xing Catalyst Co Ltd
Heesung Catalysts Corp
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Abstract

本发明涉及一种使用氨或尿素作为还原剂的选择性催化还原的催化剂，且特别涉及一种涂覆有氧化铈或氧化铈复合氧化物的选择性催化还原的催化剂。本发明涉及的催化剂，其中氧化铈或氧化铈复合氧化物涂覆到包含如钒等沸石或非沸石基底金属的选择性催化还原的催化剂的上层。令人惊奇地，如果氧化铈或含氧化铈的复合氧化物涂覆到选择性催化还原的催化剂的最上层，能够在相对较低温度显示出催化活性，能够改善耐热性和对碱金属等的抗毒性并能增加尿素水解的效率。

Description

提高耐用性的用于选择性催化还原的催化剂
技术领域
本发明涉及一种使用氨或尿素作为还原剂的选择性催化还原催化剂，该催化剂在抗毒性和耐热性方面都有所改善且低温活性得以提高，更特别涉及一种选择性催化还原催化剂，其中包含沸石或非沸石基底金属的催化剂的最上层表面涂覆有氧化铈或氧化铈复合氧化物，其中用氧化铈或氧化铈复合氧化物涂覆催化剂的最上层表面能使氮氧化物（NOx）的还原性能在相对低温的范围内得以提高，并能改善因碱金属组分如磷、钙、锌等以及内燃机排出废气中未燃烃所引起的中毒的耐用性，且即使暴露在高温也能提高耐热性。此外，在选择性催化还原时使用尿素作为还原剂可增加尿素水解的效率，从而提高了氨产率。
背景技术
就使用化学计量燃烧所需预定量或预定量以上的空气的情况下，也就是在稀燃条件下下运行的内燃机而论，很难从废气中去除氮氧化物（NOx）。
在应用于对应稀燃条件的固定源且其效果已证实的NOx还原工艺中，这种工艺之一是使用氨或氨水的选择性催化还原（SCR）。这样，NOx与还原剂氨在SCR催化剂的表面上反应并因而还原成氮气（N2），由此减少NOx的量。通常，钒钛氧化物已经被用作固定源中的SCR催化剂。在这种情况下，300~450℃具有90%或以上的NOx还原性能。为了将钒钛氧化物催化剂应用到移动源，研制了包含氧化钨（WO3）等的催化剂，以使由于因燃料的硫组分和高温暴露引起的中毒而降低的催化性能得以改善，且它们正被应用于大的柴油车辆。为了配合将来船运业中加强的废气规定，预期将会频繁使用钒钛氧化物催化剂。然而，催化剂的性能会由于高温暴露或因为废气的未燃烃及燃料（机油）中其他碱金属组分如硫、磷、钙、锌等吸附在催化剂上而彻底地降低，这亟待解决。
另一方面，出于确保最终使用需要相比钒钛氧化物催化剂更高的温度耐用性（600℃或更高）和更高的活化温度（350~550℃）的目的，研制并已经使用了沸石催化剂如Fe-β、Cu-β、Fe-ZSM5和Cu-ZSM5催化剂，其中ZSM5和β-沸石与过渡金属离子如铁（Fe）或铜（Cu）进行离子交换。但是，这些催化剂存在一些问题，因为低温活性要次于钒钛氧化物催化剂且在因烃类和碱金属组分如硫、磷、钙、锌等引起中毒时催化性能会显著降低。
根据全球温室气体减排和废气排放管理的要求，新近正研制的内燃机被广泛地经受低温燃烧工艺以获得高的燃料效率和废气减排。因此，废气温度预期在将来将会更低，这样，低温性能是受到大量关注的一个特性。
发明内容
技术问题
因此，现在对具有优良的低温活性、耐内燃机中高温暴露的耐热性以及抗因碱金属组分如硫、磷、钙、锌等引起中毒的抗毒性的新型催化剂存在需求。
本发明人使用氧化铈或氧化铈复合氧化物作为传统SCR催化剂的最上层来进行SCR反应，并因而发现获得的催化剂能够解决上述问题，此外发现，最高涂层的存在可提高尿素向氨的转变，这些发现使得本发明得以完成。
技术方案
本发明提供了一种包含(a)沸石或非沸石作为基底金属（钒钛氧化物和氧化锆）的SCR催化剂，其中，其最上层包含氧化铈或氧化铈复合氧化物。
本发明中，复合氧化物是包含含有铈的两种或两种以上元素的混合氧化物，特别是非物理混合的、包含含有铈的两种或两种以上元素的氧化物的非晶氧化物。例如，复合氧化物可以是Ce-LMNOx(L、M、N=Zr、Y、Pr、Nd、La或Mn)。
单独的氧化铈或氧化铈复合氧化物可涂覆到包含沸石或非沸石作为基底金属（钒钛氧化物和氧化锆）的常规SCR催化剂上。
本发明的SCR催化剂可涂覆到陶瓷蜂窝体上或可挤压成蜂窝形状。因此，本发明的氧化物涂层可经由典型的湿涂法（wash-coating process）通过能够商业上使用该蜂窝的氧化铈基湿涂溶液来完成。为了获得平坦的SCR催化剂层，湿涂工艺包括利用湿涂溶液浸涂包含沸石或非沸石的SCR催化剂并使用压缩空气去除过量的氧化物涂层。湿涂催化剂可在大约100℃下干燥，然后在450~550℃煅烧。
有益效果
根据本发明，当具有氧化铈涂层的SCR催化剂应用到氨/尿素-SCR系统时，能够获得优良的低温活性，并能加快尿素水解，从而提高废气中NOx的转化率。此外，该催化剂在高温暴露时具有耐热性，并增加了抗毒性，这使得它即使在暴露于高浓度的硫或碱金属时，也能保持催化活性。
附图说明
图1例示了在将标准催化剂（没有氧化铈涂层）和研制的催化剂（具有氧化铈涂层）使用航运燃料（MF30）长时间暴露于有毒组分后催化剂（标准催化剂、研制的催化剂）的NOx的转化率。
图2例示了在625℃下水热处理24小时后标准催化剂或研制的SCR催化剂（钒钛氧化物催化剂）的NOx的转化率。
图3例示了在700℃下水热处理24小时后标准催化剂或研制的SCR催化剂（铁-沸石催化剂）的NOx转化率。
图4例示了标准催化剂或研制的SCR催化剂（钒钛氧化物催化剂）的尿素水解效率。
具体实施方式
实施例1
研制的催化剂A以如下方式加以制备，将圆柱形的蜂窝状载体(110Φ*78.9、400cpsi、0.75L)涂覆钒钛氧化物，然后浸入到仅包含氧化铈的湿涂溶液中，以便SCR催化剂的最上层形成有氧化铈涂层。制备的催化剂在10%湿度条件下于625℃进行24小时水热处理。
实施例2
研制的催化剂B以如下方式加以制备，将六面体的蜂窝状载体(150*150*100、36cpsi、2.25L)涂覆钒钛氧化物，然后浸入到包含主要由氧化铈组成的复合氧化物的湿涂溶液中，以便SCR催化剂的最上层形成有氧化铈涂层。制备的（新制的）催化剂使用船运燃料MF30（35%柴油机+65%船用燃料油C）于250℃下老化8小时。
实施例3
研制的催化剂C以如下方式加以制备，将圆柱形的蜂窝状载体(110Φ*78.9、400cpsi、0.75L)涂覆铁-沸石，然后浸入到仅包含氧化铈的湿涂溶液中，以便SCR催化剂的最上层形成有氧化铈涂层。制备的催化剂在10%湿度条件下于700℃下进行24小时水热处理。
测试实施例1
SCR催化剂的低温活性测试
为了评价SCR催化剂的活性，实施例1、2和3中每个涂覆的蜂窝状载体都放入到测试反应器中。在涂覆到六面体载体上的SCR催化剂的情况下，NOx（350~400ppm）以20,000/小时空间速度供入（经由入口），在涂覆到圆柱形载体上的SCR催化剂的情况下，NOx（400~450ppm）以53,000/小时的空间速度供入，并测量和比较了NOx的转化率。
NOx的转化结果显示在图1（使用船运燃料老化的催化剂），图2（在625℃下进行水热处理的催化剂）和图3（在700℃下进行水热处理的催化剂）中。如图1中所示，与没有氧化物涂层的SCR催化剂（标准催化剂）相比，具有氧化铈涂层作为最上层的SCR催化剂（研制的催化剂）即使在低温（200~250℃）使用船运燃料进行老化处理后也具有更高的转化率。如图2和3中所示，与没有氧化物涂层的SCR催化剂（标准催化剂）相比，具有氧化铈涂层作为最上层的SCR催化剂（研制的催化剂）在水热处理后，具有更高的NOx转化率。
测试实施例2
尿素水解性能测试
为了评价SCR催化剂的活性，将实施例1中涂覆有SCR催化剂的每个蜂窝状载体放入测试反应器中，然后以53,000/小时的空间速度喷射尿素（2g/分），然后测量并比较尿素转化成氨的水解转化率。
氨转化率结果显示在图4中。如图4中所示，具有氧化铈涂层作为最上层的SCR催化剂与没有氧化物涂层的SCR催化剂相比，具有更高的尿素水解转化率。
工业实用性
因此，当将本发明的具有氧化铈涂层的SCR催化剂应用到尿素-SCR系统时，能够获得优良的低温活性，并能加快尿素水解，从而改善总体NOx转化率。

Claims (5)

1.一种选择性催化还原（SCR）的催化剂，包含仅由氧化铈或由氧化铈复合氧化物组成的最上层。
2. 权利要求1所述的选择性催化还原（SCR）的催化剂，其中所述SCR催化剂包含沸石或非沸石作为基底金属氧化物。
3. 权利要求2所述的选择性催化还原（SCR）的催化剂，其中所述非沸石基底金属氧化物是钒钛氧化物或氧化锆。
4. 权利要求1所述的选择性催化还原（SCR）的催化剂，其中氧化铈复合氧化物是铈和选自稀土金属、过渡金属、碱金属与碱土金属中的一种或多种金属的混合氧化物。
5. 权利要求1所述的选择性催化还原（SCR）的催化剂，其中所述SCR催化剂应用到蜂窝体上或挤压成蜂窝形状。
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