CN110124659B - 一种铈锆铝基复合材料、cGPF催化剂及其制备方法 - Google Patents

一种铈锆铝基复合材料、cGPF催化剂及其制备方法 Download PDF

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CN110124659B
CN110124659B CN201910538169.5A CN201910538169A CN110124659B CN 110124659 B CN110124659 B CN 110124659B CN 201910538169 A CN201910538169 A CN 201910538169A CN 110124659 B CN110124659 B CN 110124659B
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zirconium
cerium
composite material
aluminum
catalyst
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CN110124659A (zh
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陈山虎
李大成
兰丽
王金凤
黄超谋
叶辉
刘屿剑
杨兰
张锋
杨怡
程永香
颜意
董银华
王云
李云
陈启章
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Sinocat Environmental Technology Co Ltd
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Sinocat Environmental Technology Co Ltd
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Priority to CN201910538169.5A priority Critical patent/CN110124659B/zh
Publication of CN110124659A publication Critical patent/CN110124659A/zh
Priority to PCT/CN2020/096584 priority patent/WO2020253726A1/zh
Priority to US17/619,391 priority patent/US20220363603A1/en
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Abstract

本发明公开了一种铈锆铝基复合材料、cGPF催化剂及其制备方法；本发明采用分步沉淀的方法先制备铝基预处理材料，再将其与锆、铈溶胶共沉淀，最后经过高温焙烧得到铈锆铝基复合材料，该铈锆铝基复合材料具有更好的致密性，密度更大，将其用于cGPF催化剂中时，占据的催化剂载体上孔道的体积更小，使cGPF催化剂具有更低的背压和更好的抗灰分累积能力，有利于cGPF催化剂的大规模应用。

Description

一种铈锆铝基复合材料、cGPF催化剂及其制备方法
技术领域
本发明涉及尾气净化材料领域，具体涉及一种铈锆铝基复合材料、cGPF催化剂及其制备方法。
背景技术
汽油机尾气排放物是构成中国城市污染的主要来源之一，汽油机发动机排放的尾气中主要污染物为一氧化碳（CO）、碳氢化合物（HC）、氮氧化合物（NOX）和颗粒物（PM）等。随着能源和环境问题的日趋紧迫，为了保护环境，中国对机动车尾气的排放提出了更高的要求，中国即将在2020年实施国6排放标准，而不少区域甚至将法规提前至2019年开始实施。国6排放标准将尾气中颗粒物的浓度作为了重要限定标准，因而，控制尾气中颗粒物的浓度成为今后汽油机发动机尾气净化的重点。然而，传统的三效催化剂（TWC）只能有效的净化尾气中的CO、HC和NOX，却不能控制尾气中颗粒物的浓度，由此可以预见，能显著降低尾气中颗粒物的浓度的汽油机颗粒捕集器催化剂（cGPF）将会被大规模推广使用。
汽油机发动机颗粒物的组成虽然复杂，但其中的大部分组分都可以通过燃烧去除（如cGPF催化剂），进而实现对颗粒物的排放浓度控制，使汽油机发动机尾气达到国6的排放标准。然而，颗粒物中的碳烟(Soot)等组分燃烧后仍然会有一部分最终转化为不可燃烧去除的灰分(Ash)，并沉积在cGPF催化剂孔道内，造成催化剂背压升高和性能下降，最终导致cGPF催化剂失效或发生安全风险。因此，提高cGPF催化剂的抗高灰分累积能力，是降低催化剂背压并保持催化性能，降低安全风险的必要保障。
现今的cGPF催化剂中催化剂涂层大多是采用混合的铈锆基材料和氧化铝基材料，虽然其对汽油机发动机颗粒物具有优异的净化效果，从而能有效控制颗粒物的排放浓度，使汽油机发动机尾气符合国6的排放标准，但由于其密度小，体积大，在将其填充到cGPF载体孔道后，会占据孔道较大的体积，从而减小孔道孔径和孔容，导致催化剂背压升高，抗灰分累积能力下降，不利于cGPF催化剂的大规模应用。
发明内容
本发明的目的在于克服现有cGPF催化剂中的铈锆基材料和氧化铝基材料占用催化剂载体孔道体积过大而导致cGPF催化剂抗灰分累积能力差的缺陷，提出一种铈锆铝基复合材料、cGPF催化剂及其制备方法；本发明采用分步沉淀的方法先制备铝基预处理材料，再将其与锆、铈溶胶共沉淀，最后经过高温焙烧得到铈锆铝基复合材料，该铈锆铝基复合材料具有更好的致密性，密度更大，将其用于cGPF催化剂中时，占据的催化剂载体上孔道的体积更小，使cGPF催化剂具有更低的背压和更好的抗灰分累积能力，有利于cGPF催化剂的大规模应用。
为了实现上述发明目的，本发明提供了一种铈锆铝基复合材料的制备方法，包括以下步骤：
（1）将拟薄水铝石用柠檬酸水溶液溶解后，再用氨水调节pH值到4-10，搅拌反应完成后，过滤、干燥得到沉淀物；将沉淀物在200-400℃的温度下进行焙烧处理0.1-5h，得到预处理材料；所述拟薄水铝石与柠檬酸的质量之比为5-20︰1；
（2）将预处理材料加入到混合溶胶溶液中，溶解完成后，再用氨水调节pH值到4-10，搅拌反应完成后，过滤、干燥得到混合物沉淀；所述的混合溶胶为含有含铈离子和锆离子的溶胶；
（3）将混合物沉淀先在500-600℃的温度下焙烧1-10h，再在800-1100℃温度下焙烧1-10h，得到铈锆铝基复合材料。
优选的，步骤（1）中，所述的柠檬酸水溶液中，柠檬酸的质量分数为5-20%,；优选的柠檬酸质量分数，反应速度快，反应更彻底。
优选的，步骤（1）和（2）中所述的氨水浓度为20-30wt%；优选的氨水浓度，反应速度可控，反应时间更短，得到的铈锆铝基复合材料对尾气的催化净化效果更好。
优选的，步骤（1）和（2）中的干燥温度为60-150℃，时间为1-12h；优选的干燥温度和时间，干燥速度更快，能耗更低，也不会导致干燥物因高温而发生化学反应。
优选的，步骤（2）中的混合溶胶为还含有钇离子、镧离子、钕离子、镨离子、钯离子、锶离子中一种或几种的溶胶；优选的混合溶胶含有更多的稀土金属元素，密度更小，制备得到的铈锆铝基复合材料对尾气的催化净化效果更好。
为了实现上述发明目的，进一步的，本发明提供了一种铈锆铝基复合材料，该铈锆铝基复合材料是通过上述制备方法制备得到的。
优选的，所述的铈锆铝基复合材料包括以下组分：4-30wt% 的CeO2、1-30wt% 的ZrO2、40-95wt% 的Al2O3和0-20wt%的稀土金属氧化物；最优选的，所述的铈锆铝基复合材料包括以下组分：10-20wt% 的CeO2、5-15wt% 的ZrO2、60-75wt% 的Al2O3和5-10wt%的稀土金属氧化物；所述的稀土金属氧化物包括Y2O3、La2O3、Nd2O3、Pr6O11、BaO、SrO中的一种或几种；材料的组成影响材料的性能，优选的铈锆铝基复合材料组成，比表面积更大，孔容更大，密度更大，更有利于减小涂层对催化剂载体上孔道体积的占据，从而更好的降低催化剂背压，提高抗灰分累积能力，对尾气的催化净化效果也会更好。
优选的，所述的铈锆铝基复合材料比表面为50-200 m2/g；最优选的，所述的铈锆铝基复合材料比表面为80-120 m2/g；材料比表面积与密度成反比，而比表面积越大，与尾气的接触面越大，催化净化效果越好，但材料密度越小，涂层对催化剂载体孔洞的占比会越大，抗灰分累积能力越差，优选的铈锆铝基复合材料比表面，能使催化剂在对尾气的催化净化效果好的同时，保证抗灰分累积能力也很好。
优选的，所述的铈锆铝基复合材料孔容为0.2-2.0 ml/g；最优选的，所述的铈锆铝基复合材料孔容为0.4-1.5 ml/g；材料孔容与密度成反比，而孔容越大，与尾气的接触面越大，催化净化效果越好，但密度越小，对催化剂载体孔洞的占比越大，抗灰分累积能力越差，优选的铈锆铝基复合材料孔容，能使催化剂在对尾气的催化净化效果好的同时，保证抗灰分累积能力也很好。
优选的，所述的铈锆铝基复合材料的密度为0.5-1.5g/ml；最优选的，所述的铈锆铝基复合材料的密度为0.8-1.2ml/g；材料的密度与孔容和比表面积成反比，而密度越大，对催化剂载体孔洞的占比越小，抗灰分累积能力越好，但密度越大，比表面积和孔容就越小，与尾气的接触面越小，催化净化效果越差，优选的铈锆铝基复合材料密度，能使催化剂在抗灰分累积能力很好的同时，对尾气的催化净化效果也好。
更进一步的，本发明提供了一种cGPF催化剂，所述cGPF催化剂的催化剂涂层中含有上述铈锆铝基复合材料。
更进一步的，本发明提供了一种cGPF催化剂的制备方法，包括以下步骤：
（1）制备浆料：将铈锆铝基复合材料、铈锆基材料、铝溶胶和去离子水混合球磨后，加入造孔剂，混合球磨后，再加入钯盐溶液和铑盐溶液，混合球磨得到涂层浆料；
（2）涂覆：将涂层浆料涂覆在催化剂载体上；
（3）焙烧：将涂覆好的催化剂载体进行干燥、焙烧，得到cGPF催化剂。
其中，优选的，步骤（1）中所述的铈锆基材料中包括20-80wt%的CeO2、10-70wt%的ZrO2和0-10wt%的稀土金属氧化物；所述的稀土金属氧化物包括Y2O3、La2O3、Nd2O3、Pr6O11、BaO、SrO中的一种或几种；优选的铈锆基材料的催化性能更好，得到的cGPF催化剂综合性能更好。
其中，优选的，步骤（1）中所述的铈锆铝基复合材料与铈锆基材料的质量比为1︰3-3︰1；优选的铈锆铝基复合材料与铈锆基材料的质量比，能使催化剂在抗灰分累积能力很好的同时，对尾气的催化净化效果也好。
其中，优选的，步骤（1）中铝溶胶的用量为浆料总质量的1-5%；优选的铝溶胶用量，涂层不易脱落，能使催化剂在抗灰分累积能力很好的同时，对尾气的催化净化效果也好。
其中，优选的，步骤（1）中造孔剂的用量为浆料质量的1-20%；优选的造孔剂用量，造孔效果好，催化剂涂层的密度较小，能使催化剂在抗灰分累积能力很好的同时，对尾气的催化净化效果也好。
其中，优选的，所述的造孔剂为聚醚、聚酯、聚酰胺、聚氨酯、纤维素、糖类、聚乙烯、聚苯乙烯中的一种或几种；优选的造孔剂造孔效果好，对cGPF催化剂的抗灰分累积能力影响作用小。
其中，优选的，步骤（1）中，涂层浆料的粒度D50不高于5μm；最优选的，所述的涂层浆料的粒度D50为2-3μm；优选的涂层浆料粒度，涂覆性好，涂覆更均匀。
其中，优选的，步骤（1）中，涂层浆料的固含量为20-40wt%；优选的涂层浆料固含量，涂覆性好，涂覆更均匀。
其中，优选的，步骤（2）中，涂层浆料的涂覆量为20-140g/L；最优选的，涂层浆料的涂覆量为60-100 g/L；优选的涂覆量，占据的催化剂载体孔容较小的同时，又能保证催化剂涂层厚度，使催化剂在抗灰分累积能力很好的同时，对尾气的催化净化效果也好。
其中，优选的，步骤（3）中，干燥温度为90-150℃，干燥时间为3-10h；优选的干燥温度，能耗低，时间段，不影响涂层的粘附性。
其中，优选的，步骤（3）中，焙烧的温度为500-600℃，焙烧的时间为1-4h；优选的焙烧温度，能耗低，时间短，催化剂性能稳定。
与现有技术相比，本发明的有益效果：
1、本发明制备方法利用分步沉淀与共沉淀相结合的方法，使铈锆铝基复合材料的致密性增加，制备得到的铈锆铝基复合材料的密度更小。
2、本发明制备得到的铈锆铝基复合材料用于cGPF催化剂，能减小占用催化剂载体孔道的体积，从而降低cGPF催化剂的背压，增加cGPF催化剂的抗灰分累积能力。
3、本发明铈锆铝基复合材料的制备方法简单、可靠，适用于铈锆铝基复合材料的大规模生产。
4、本发明cGPF催化剂中含有的铈锆铝基复合材料密度更大，占用的催化剂载体孔道体积小，背压更低，抗灰分累积能力更强。
5、本发明cGPF催化剂的制备方法简单、可靠，适用于cGPF催化剂的大规模生产。
具体实施方式
下面结合试验例及具体实施方式对本发明作进一步的详细描述。但不应将此理解为本发明上述主题的范围仅限于以下的实施例，凡基于本发明内容所实现的技术均属于本发明的范围。
实施例1
一种铈锆铝基复合材料，由以下组分构成：20%CeO2、25%ZrO2、2.5%La2O3、2.5%Y2O3、50%Al2O3，制备方法如下：
（1）将拟薄水铝石用质量分数为10%的柠檬酸水溶液溶解后，再用氨水调节pH值到7，搅拌反应完成后，过滤、干燥得到沉淀物；将沉淀物在300℃的温度下进行焙烧处理3h，得到预处理材料；
（2）将预处理材料加入到铈、锆、镧、钇的混合溶胶溶液中，溶解完成后，再用氨水调节pH值到7，搅拌反应完成后，过滤、干燥得到混合物沉淀；
（3）将混合物沉淀先在550℃的温度下焙烧5h，再在1000℃温度下焙烧3h，得到铈锆铝基复合材料；
经检测，该铈锆铝基复合材料的比表面为76.2m2/g，孔容为0.8ml/g，密度为1.23g/ml。
实施例2
一种铈锆铝基复合材料，由以下组分构成：20%CeO2、25%ZrO2、2.5%La2O3、2.5%Y2O3、50%Al2O3，制备方法如下：
（1）将拟薄水铝石用质量分数为5%的柠檬酸水溶液溶解后，再用氨水调节pH值到4，搅拌反应完成后，过滤、干燥得到沉淀物；将沉淀物在200℃的温度下进行焙烧处理5h，得到预处理材料；
（2）将预处理材料加入到铈、锆、镧、钇的混合溶胶溶液中，溶解完成后，再用氨水调节pH值到4，搅拌反应完成后，过滤、干燥得到混合物沉淀；
（3）将混合物沉淀先在500℃的温度下焙烧10h，再在1100℃温度下焙烧1h，得到铈锆铝基复合材料；
经检测，该铈锆铝基复合材料的比表面为74.8m2/g，孔容为0.73ml/g，密度为1.25g/ml。
实施例3
一种铈锆铝基复合材料，由以下组分构成：20%CeO2、25%ZrO2、2.5%La2O3、2.5%Y2O3、50%Al2O3，制备方法如下：
（1）将拟薄水铝石用质量分数为15%的柠檬酸水溶液溶解后，再用氨水调节pH值到10，搅拌反应完成后，过滤、干燥得到沉淀物；将沉淀物在400℃的温度下进行焙烧处理0.1h，得到预处理材料；
（2）将预处理材料加入到铈、锆、镧、钇的混合溶胶溶液中，溶解完成后，再用氨水调节pH值到10，搅拌反应完成后，过滤、干燥得到混合物沉淀；
（3）将混合物沉淀先在600℃的温度下焙烧1h，再在800℃温度下焙烧10h，得到铈锆铝基复合材料；
经检测，该铈锆铝基复合材料的比表面为78.5m2/g，孔容为0.83ml/g，密度为1.21g/ml。
实施例4
一种铈锆铝基复合材料，由以下组分构成：10%CeO2、10%ZrO2、2.5%La2O3、2.5%Y2O3、75%Al2O3，制备方法如下：
（1）将拟薄水铝石用质量分数为12%的柠檬酸水溶液溶解后，再用氨水调节pH值到7，搅拌反应完成后，过滤、干燥得到沉淀物；将沉淀物在300℃的温度下进行焙烧处理3h，得到预处理材料；
（2）将预处理材料加入到铈、锆、镧、钇的混合溶胶溶液中，溶解完成后，再用氨水调节pH值到7，搅拌反应完成后，过滤、干燥得到混合物沉淀；
（3）将混合物沉淀先在550℃的温度下焙烧5h，再在1000℃温度下焙烧3h，得到铈锆铝基复合材料；
经检测，该铈锆铝基复合材料的比表面为92.3m2/g，孔容为0.89ml/g，密度为1.13g/ml。
实施例5
一种铈锆铝基复合材料，由以下组分构成：10%CeO2、10%ZrO2、2.5%La2O3、2.5%Y2O3、75%Al2O3，制备方法如下：
（1）将拟薄水铝石用质量分数为10%的柠檬酸水溶液溶解后，再用氨水调节pH值到4，搅拌反应完成后，过滤、干燥得到沉淀物；将沉淀物在200℃的温度下进行焙烧处理5h，得到预处理材料；
（2）将预处理材料加入到铈、锆、镧、钇的混合溶胶溶液中，溶解完成后，再用氨水调节pH值到4，搅拌反应完成后，过滤、干燥得到混合物沉淀；
（3）将混合物沉淀先在500℃的温度下焙烧10h，再在1100℃温度下焙烧1h，得到铈锆铝基复合材料；
经检测，该铈锆铝基复合材料的比表面为91.8m2/g，孔容为0.87ml/g，密度为1.14g/ml。
实施例6
一种铈锆铝基复合材料，由以下组分构成：10%CeO2、10%ZrO2、2.5%La2O3、2.5%Y2O3、75%Al2O3，制备方法如下：
（1）将拟薄水铝石用质量分数为20%的柠檬酸水溶液溶解后，再用氨水调节pH值到10，搅拌反应完成后，过滤、干燥得到沉淀物；将沉淀物在400℃的温度下进行焙烧处理0.1h，得到预处理材料；
（2）将预处理材料加入到铈、锆、镧、钇的混合溶胶溶液中，溶解完成后，再用氨水调节pH值到10，搅拌反应完成后，过滤、干燥得到混合物沉淀；
（3）将混合物沉淀先在600℃的温度下焙烧1h，再在800℃温度下焙烧10h，得到铈锆铝基复合材料；
经检测，该铈锆铝基复合材料的比表面为95.3m2/g，孔容为0.91ml/g，密度为1.11g/ml。
对比例1
一种铈锆铝复合材料，直接由20%CeO2、25%ZrO2、2.5%La2O3、2.5%Y2O3和50%Al2O3混合而成。
经检测，该铈锆铝复合材料的比表面为103.2m2/g，孔容为0.97ml/g，密度为1.06g/ml。
对比例2
一种铈锆铝基复合材料，由以下组分构成：20%CeO2、25%ZrO2、2.5%La2O3、2.5%Y2O3、50%Al2O3，制备方法如下：
（1）将拟薄水铝石用质量分数为10%的柠檬酸水溶液溶解后，加入到铈、锆、镧、钇的混合溶胶溶液中，溶解完成后，再用氨水调节pH值到7，搅拌反应完成后，过滤、干燥得到混合物沉淀；
（2）将混合物沉淀先在550℃的温度下焙烧5h，再在1000℃温度下焙烧3h，得到铈锆铝基复合材料；
经检测，该铈锆铝基复合材料的比表面为93.7m2/g，孔容为0.90ml/g，密度为1.12g/ml。
对比例3
一种铈锆铝基复合材料，由以下组分构成：20%CeO2、25%ZrO2、2.5%La2O3、2.5%Y2O3、50%Al2O3，制备方法如下：
（1）将拟薄水铝石用质量分数为10%的柠檬酸水溶液溶解后，再用氨水调节pH值到7，搅拌反应完成后，过滤、干燥得到沉淀物；将沉淀物在300℃的温度下进行焙烧处理3h，得到预处理材料；
（2）将铈、锆、镧、钇的混合溶胶溶液用氨水调节pH值到7，搅拌反应完成后，过滤、干燥得到混合物沉淀；
（3）将混合物沉淀和预处理材料混合均质后，先在550℃的温度下焙烧5h，再在1000℃温度下焙烧3h，得到铈锆铝基复合材料；
经检测，该铈锆铝基复合材料的比表面为96.8m2/g，孔容为0.93ml/g，密度为1.09g/ml。
对比例4
一种铈锆铝复合材料，直接由10%CeO2、10%ZrO2、2.5%La2O3、2.5%Y2O3、75%Al2O3混合而成。
经检测，该铈锆铝复合材料的比表面为134.3m2/g，孔容为1.31ml/g，密度为0.83g/ml。
对比例5
一种铈锆铝基复合材料，由以下组分构成：10%CeO2、10%ZrO2、2.5%La2O3、2.5%Y2O3、75%Al2O3，制备方法如下：
（1）将拟薄水铝石用质量分数为10%的柠檬酸水溶液溶解后，加入到铈、锆、镧、钇的混合溶胶溶液中，溶解完成后，再用氨水调节pH值到7，搅拌反应完成后，过滤、干燥得到混合物沉淀；
（2）将混合物沉淀先在550℃的温度下焙烧5h，再在1000℃温度下焙烧3h，得到铈锆铝基复合材料；
经检测，该铈锆铝基复合材料的比表面为125.7m2/g，孔容为1.26ml/g，密度为0.87g/ml。
对比例6
一种铈锆铝基复合材料，由以下组分构成：10%CeO2、10%ZrO2、2.5%La2O3、2.5%Y2O3、75%Al2O3，制备方法如下：
（1）将拟薄水铝石用质量分数为10%的柠檬酸水溶液溶解后，再用氨水调节pH值到7，搅拌反应完成后，过滤、干燥得到沉淀物；将沉淀物在300℃的温度下进行焙烧处理3h，得到预处理材料；
（2）将铈、锆、镧、钇的混合溶胶溶液用氨水调节pH值到7，搅拌反应完成后，过滤、干燥得到混合物沉淀；
（3）将混合物沉淀和预处理材料混合均质后，先在550℃的温度下焙烧5h，再在1000℃温度下焙烧3h，得到铈锆铝基复合材料；
经检测，该铈锆铝基复合材料的比表面为128.4m2/g，孔容为1.28ml/g，密度为0.85g/ml。
催化剂的制备：
（1）制备浆料：将铈锆铝基复合材料（由实施例1-6或对比例1-6中制备得到）、铈锆基材料（40%CeO2、50%ZrO2、5%La2O3、5%Y2O3）按1：1混合，然后加入铝溶胶（占浆料含量的2%）、聚氨酯（占浆料含量的5%）和去离子水，加入硝酸钯溶液（保证涂层中Pd的含量密度为5g/ft3），球磨搅拌5min；加入硝酸铑溶液（保证涂层中Rh的含量密度为 5g/ft3），球磨搅拌5min，制备得到涂层浆料，控制浆料的粒度D50为2.4μm，固含量为33wt%；
（2）涂覆：将涂层浆料涂覆在壁流式堇青石载体上，涂覆高度为载体高度的90%，涂覆量50g/L
（3）焙烧：将涂覆好的催化剂载体在马弗炉中120℃干燥3h，然后在马弗炉中550℃焙烧3h，得到cGPF催化剂。
实验例：
台架灰分加载试验：
将上述制备得到的cGPF催化剂分别安装于1.8L TGDI发动机上按GB18352.6-2016轻型汽车污染物排放限值及测量方法（中国第六阶段）中的SBC循环工况进行灰分加载，采用机油掺烧方法，加载时循环最高床层温度980℃，灰分目标加载量为30g/L。
整车WLTC排放测试试验：
将上述制备得到的cGPF催化剂分别作为底盘催化剂，另外选用TWC催化剂(Φ118.4*100-750/2，Pd=103g/ft3，Rh=8g/ft3)作为紧耦合催化剂组成后处理***，在一款1.6TGDI车进行排放试验。按照“GB18352.6-2016 轻型汽车污染物排放限值及测量方法（中国第六阶段）”进行I型排放试验。另外在cGPF催化剂的入口和出口安装压力管检测WLTC循环下的背压。催化剂在1800s下的循环排放结果和最高背压差值ΔP记录如下：
编号 CO (g/km) THC (g/km) NO<sub>x</sub> (g/km) PN (个/km) ΔP (kpa)
实施例1 0.220 0.033 0.037 2.4*10<sup>11</sup> 10.5
实施例2 0.218 0.031 0.036 2.3*10<sup>11</sup> 10.1
实施例3 0.223 0.034 0.038 2.4*10<sup>11</sup> 10.8
实施例4 0.224 0.038 0.040 2.1*10<sup>11</sup> 12.3
实施例5 0.226 0.037 0.039 2.0*10<sup>11</sup> 11.8
实施例6 0.225 0.039 0.041 2.1*10<sup>11</sup> 12.7
对比例1 0.358 0.045 0.044 1.5*10<sup>11</sup> 14.5
对比例2 0.355 0.044 0.043 1.5*10<sup>11</sup> 14.4
对比例3 0.361 0.046 0.045 1.6*10<sup>11</sup> 14.7
对比例4 0.372 0.048 0.050 1.2*10<sup>11</sup> 18.2
对比例5 0.371 0.047 0.049 1.3*10<sup>11</sup> 17.5
对比例6 0.369 0.048 0.049 1.3*10<sup>11</sup> 17.9
通过上述实验数据可知，将实施例1-6中采用本发明方法制备得到的密度更大的铈锆铝基复合材料用于cGPF催化剂后，得到的cGPF催化剂在加载灰分后，其背压显著低于常规材料的cGPF催化剂，其对尾气的净化效果也更好，因而，本发明方法制备得到的铈锆铝基复合材料能显著提高cGPF催化剂的抗灰分累积能力，有利于cGPF催化剂的大规模生产和应用。而对比例1-3与实施例1、对比例4-6与实施例3中制备得到的铈锆铝基复合材料相比，对比例中的铈锆铝基复合材料密度显著降低，从而在应用于cGPF催化剂中时，会占据催化剂载体上孔隙的更多体积，从而使采用实施例铈锆铝基复合材料制备得到的cGPF催化剂的孔隙率高于对比例，cGPF催化剂的动态传质更好，对尾气的净化能力更好，对尾气中颗粒物的捕捉能力下降。

Claims (9)

1.一种铈锆铝基复合材料的制备方法，其特征在于，包括以下步骤：
（1）将拟薄水铝石用柠檬酸水溶液溶解后，再用氨水调节pH值到4-10，搅拌反应完成后，过滤、干燥得到沉淀物；将沉淀物在200-400℃的温度下进行焙烧处理0.1-5h，得到预处理材料；所述拟薄水铝石与柠檬酸的质量之比为5-20︰1；
（2）将预处理材料加入到混合溶胶溶液中，溶解完成后，再用氨水调节pH值到4-10，搅拌反应完成后，过滤、干燥得到混合物沉淀；所述的混合溶胶为含有铈离子和锆离子的溶胶；所述混合溶胶为还含有钇离子、镧离子、钕离子、镨离子、锶离子中一种或几种；
（3）将混合物沉淀先在500-600℃的温度下焙烧1-10h，再在800-1100℃温度下焙烧1-10h，得到铈锆铝基复合材料。
2.一种铈锆铝基复合材料，其特征在于，通过权利要求1所述制备方法制备得到。
3.根据权利要求2所述的复合材料，其特征在于，所述的铈锆铝基复合材料包括以下组分：4-30wt% 的CeO2、1-30wt% 的ZrO2、40-95wt% 的Al2O3和5-20wt%的稀土金属氧化物；所述稀土金属氧化物包括Y2O3、La2O3、Nd2O3、Pr6O11、SrO中的一种或几种。
4.根据权利要求2所述的复合材料，其特征在于，所述的铈锆铝基复合材料比表面为50-200 m2/g。
5.根据权利要求2所述的复合材料，其特征在于，所述的铈锆铝基复合材料孔容为0.2-2.0 mL/g。
6.根据权利要求2所述的复合材料，其特征在于，所述的铈锆铝基复合材料的密度为0.5-1.5g/mL。
7.一种cGPF催化剂，其特征在于，所述cGPF催化剂的催化剂涂层中含有权利要求2-6任一项所述的铈锆铝基复合材料。
8.一种如权利要求7所述cGPF催化剂的制备方法，其特征在于，包括以下步骤：
（1）制备浆料：将铈锆铝基复合材料、铈锆基材料、铝溶胶和去离子水混合球磨后，加入造孔剂，混合球磨后，再加入钯盐溶液和铑盐溶液，混合球磨得到涂层浆料；
（2）涂覆：将涂层浆料涂覆在催化剂载体上；
（3）焙烧：将涂覆好的催化剂载体进行干燥、焙烧，得到cGPF催化剂。
9.根据权利要求8所述的制备方法，其特征在于，步骤（1）中所述的铈锆铝基复合材料与铈锆基材料的质量比为1︰3-3︰1。
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