CN101842155A - 用于处理柴油lng双燃料机动车的废气的催化剂 - Google Patents
用于处理柴油lng双燃料机动车的废气的催化剂 Download PDFInfo
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Abstract
本发明涉及用于处理柴油LNG双燃料机动车的废气的催化剂,其中浸渍有作为催化剂活性成分的钯和铂。用于处理柴油LNG双燃料机动车的废气的该催化剂具有优异的甲烷氧化活性和优异的防止硫中毒效果。
Description
技术领域
本发明涉及用于处理柴油LNG(液化天然气)双燃料机动车的废气的催化剂,更具体而言,涉及柴油LNG双燃料机动车的催化剂,所述催化剂可以有效地除去柴油LNG双燃料机动车的废气中所含有的甲烷并且还具有优异的硫中毒抗性。
背景技术
天然气机动车可根据燃料供给系统分为CNG(压缩天然气)型和LNG型。CNG型使用在约200个大气压的压力压缩并且储存在高压容器中的气体,而LNG型使用温度约为-130℃的低温燃料。在国内外CNG被主要用作天然气燃料的原因似乎在于,与CNG相比LNG难以应用于机动车,并且没有足够的用于提供LNG的基础设施。在韩国,CNG机动车获得了市场的良好接受并处于成熟阶段,但是LNG机动车却刚刚通过开发阶段且正处于试驾阶段。
此外,根据点火系统,天然气发动机可以分为专用型和双燃料型。专用型利用电点火系统并且主要用在汽油发动机中,而双燃料型使用柴油燃料作为点火源。当将现有汽油机动车改造为天然气机动车时,如果应用双燃料型,则可以通过仅安装天然气供给系统而不改变点火系统来比较简单地实现燃料转换。
在天然气机动车中,甲烷是废气的主要成分。甲烷是具有长寿命的潜在的温室气体,并且显示出比二氧化碳更高的温室效应。由于天然气机动车排出的甲烷存在对环境的影响,因此预计早晚会提出排放法规,并且天然气机动车的以现有状态排出的甲烷约有60%应由低温后处理装置等进行处理,以遵守最严格的欧洲法规。
近来,使用其中浸渍有作为活性成分的钯的催化剂来氧化甲烷。然而,这存在钯在硫条件下具有显著降低的催化活性的问题。
此外,对于柴油LNG双燃料机动车,由于LNG不含硫但柴油含硫,因此柴油中所含的硫会使用于氧化废气中的甲烷的催化活性材料中毒,因而需要开发用于柴油LNG双燃料机动车的除甲烷催化剂。
发明内容
技术问题
本发明的一个目的在于提供用于处理柴油LNG双燃料机动车的废气的催化剂,所述催化剂可以有效地除去柴油LNG双燃料机动车的废气中所含有的甲烷。
本发明的另一个目的在于提供用于处理柴油LNG双燃料机动车的废气的催化剂,所述催化剂具有高甲烷去除性能和优异的硫中毒抗性。
技术解决方案
本发明人从为实现上述目的而反复进行的研究的结果中发现,通过在催化剂中浸渍铂和钯同时调整铂与钯的重量比,可以控制硫中毒现象。
一般而言,在韩国,柴油燃料被控制为含有50ppm以下的硫。因此,柴油LNG双燃料机动车的废气中的硫浓度处于10ppm以下的程度,为0.1ppm~10ppm,更具体而言为0.1ppm~5ppm,但这取决于混合燃料燃烧比。在本发明中,调整钯与铂的浸渍比以便在柴油LNG双燃料机动车的废气条件中具有优异的甲烷氧化活性。结果,本发明人发现,当钯与铂的重量比为1∶0.1~0.5时具有高甲烷氧化活性和优异的硫中毒抗性。
本发明涉及用于处理柴油LNG双燃料机动车的废气的催化剂,其中,作为催化剂活性成分的钯与铂以1∶0.1~0.5的重量比浸渍,更优选的是,用于处理柴油LNG双燃料机动车的废气的催化剂具有陶瓷基质,所述陶瓷基质上沉积有经酸化处理的载体和重量比为1∶0.1~0.5的作为催化剂活性成分的钯和铂。
钯和铂的重量比优选为1∶0.1~0.5,更优选为1∶0.1~0.3。
钯具有比铂更优异的催化活性,但是硫容易使其中毒,从而使催化活性劣化。因此,除钯之外,还需提供具有防止硫中毒效果的助催化剂。铂作为具有防止硫中毒效果同时保持甲烷氧化活性的助催化剂具有优异的效果,但是与钯相比其甲烷氧化活性更低。因此,铂与钯的比例对于提供防止硫中毒效果和优异的甲烷氧化活性非常重要。此外,本发明人由反复研究的结果发现,当钯与铂的重量比为1∶0.1~0.5、更优选为1∶0.1~0.3时,其具有防止硫中毒效果并具有优异的甲烷氧化活性。如果铂相对于钯的重量比小于0.1,则防止硫中毒的效果会显著劣化,而如果铂相对于钯的重量比大于0.5,则甲烷氧化活性降低。因此,只有当将钯与铂的重量比被控制在上述范围内时,在柴油LNG双燃料机动车中才能够具有防止硫中毒效果和优异的甲烷氧化活性。
本发明的用于处理柴油LNG双燃料机动车的废气的催化剂具有陶瓷基质,所述陶瓷基质上沉积有载体和作为催化剂活性成分的钯和铂。陶瓷基质可以具有由如堇青石等耐热陶瓷材料形成的蜂窝孔体结构。载体可以包括氧化铝、氧化锆、二氧化硅、二氧化铈及其混合物,但是就催化活性方面而言更优选氧化铝。载体可以使用硫酸等酸处理。
优选的是,洗涂于陶瓷基质上的载体的量为0.5g/in3~4g/in3。若载体的量小于0.5g/in3,则催化剂性能显著劣化,若载体的量大于4g/in3,则催化剂性能不再提高并且难以制造。
此外,在本发明中,相对于载体和催化活化材料的总重,浸渍在催化剂中的催化活性材料的含量为0.1重量%~20重量%,优选为1重量%~15重量%。若该含量小于0.1重量%,则催化剂性能会显著劣化,若该含量大于20重量%,则催化剂性能不再提高并且从经济角度而言也是不利的。
根据本发明,当将载体洗涂于基质上之后,可以将催化活性材料浸渍于经洗涂的基质中。作为另外一种选择,当将催化活性材料浸渍于载体中之后,可以将浸渍有催化活性材料的载体洗涂在基质上。
用于处理柴油LNG双燃料机动车的废气的催化剂可以由包括以下步骤的方法制造:
通过将氧化铝洗涂在陶瓷基质上制备经洗涂的基质,然后干燥并煅烧该经洗涂的陶瓷基质;和
通过将经洗涂的基质浸入含有钯和铂的催化溶液中来浸渍催化剂活性成分,然后干燥并煅烧经洗涂的陶瓷基质。
用于制备催化溶液的钯前体包括硝酸钯、氯化钯和四氨基氯化钯等。铂前体包括四氨合硝酸铂(Pt(NH3)4(NO3)2)和六氯铂酸(H2PtCl6)等,但是就催化活性而言,H2PtCl6比Pt(NH3)4(NO3)2更具优势。
载体在基质上的洗涂以及干燥和煅烧可以通过本领域的典型方法来进行。
有利效果
本发明的用于处理柴油LNG双燃料机动车的催化剂具有优异的甲烷氧化活性和优异的硫中毒抗性。
附图说明
通过结合附图提供的对优选实施方式的以下描述,本发明的上述及其它目的、特征和优点将变得显而易见,附图中:
图1是显示浸渍有作为催化剂活性成分的钯和铂的甲烷氧化催化剂的活性评价结果的图。
图2是显示催化剂对于硫的抵抗性的评价结果的图。
具体实施方式
下面将参考附图详细描述本发明的实施方式。
[实施方式1~7]浸渍有Pd和Pt的催化剂的制造
将γ氧化铝粉(SASOL,德国,表面积:210m2/g,孔隙体积:0.5cc/g,比重:0.8g/cc)与乙酸和蒸馏水的混合溶液(重量比为1∶3.5)混合,然后通过使用湿式球磨机研磨12小时来制备均匀的氧化铝浆料。浆料中γ氧化铝粉的含量为50重量%,并且经研磨的γ氧化铝粉的平均粒径为3μm。
使用氧化铝浆料洗涂堇青石蜂窝孔体(lin3,400cpsi),使得洗涂的氧化铝的量为2g/in3,在120℃的温度干燥2小时,然后在550℃的温度煅烧3小时,由此制造洗涂有氧化铝的蜂窝孔体。
通过将作为钯前体的Pd(NO3)2水溶液(10重量%)和作为铂前体的H2PtCl6溶解在蒸馏水中分别制备80g催化溶液,使其各自具有如表1中所指定的含量。并且,将洗涂有氧化铝的蜂窝孔体浸入各催化溶液中1分钟,然后进行吹气处理,以除去残留的溶液。接下来,在大气压力下于120℃的温度干燥蜂窝孔体2小时,随后于600℃的温度煅烧4小时,由此制造浸渍有钯(Pd)和铂(Pt)的催化剂。
[实施方式8]
以与实施方式7相似的方式制造催化剂,不同之处在于,使用Pt(NH3)4(NO3)2作为铂前体。
表1
a:催化成分在催化溶液中的含量
[测试例1]催化活性的评价
将实施方式1~4中制造的蜂窝孔体催化剂固定在催化剂反应器中,然后进行甲烷(CH4)氧化实验。
使用MFC(质量流量控制器)将具有如表2中所指定的组成的模型气体以受控的流速混合,然后注入催化剂反应器中。模型气体的流速为13.6L/分钟,并且空速为GHSV 50,000小时-1。在催化剂反应器的内部上方和下方提供热电偶以控制和测量温度,并且反应温度为150℃~600℃,以5℃/分钟的加热速率分阶段升高温度,然后检查催化活性。通过气体分析器检测反应之后/之前NO、CO、CH4反应气体各自的浓度。
表2
成分 | 浓度 |
N2 | 平衡 |
空气 | 10% |
NO | 500ppm |
CO | 150ppm |
CH4 | 400ppm |
图1是显示浸渍有作为催化剂活性成分的钯和铂的甲烷氧化催化剂的活性评价结果的图。参考图1的结果,钯与铂的重量比为1∶0.2的实施方式4中的催化剂具有最优异的催化活性。
[测试例2]硫抗性的评价
将表3中所指定的模型气体注入实施方式5~8的催化剂中,评价500℃时甲烷随时间的转化率。结果如图2中所示。
表3
参考图2的结果,与Pd∶Pt=1∶0.5(重量比)相比,在Pd∶Pt=1∶0.2(重量比)的条件下,甲烷的转化率更高,并且甲烷的转化率随着浸渍量的增加而升高。在铂前体的催化活性方面,与Pt(NH3)4(NO3)2相比,H2PtCl6具有更优异的性质。
本领域技术人员将会理解,可以容易地利用以上描述中所公开的概念和具体实施方式作为基础来修改或设计实现本发明的同样目的的其它实施方式。本领域技术人员还将理解,这种等同的实施方式不会脱离如所附权利要求中所述的本发明的精神和范围。
工业实用性
本发明的用于处理柴油LNG双燃料机动车的催化剂具有优异的甲烷氧化活性和优异的硫中毒抗性。
Claims (6)
1.一种用于处理柴油LNG双燃料机动车的废气的催化剂,其中,将作为催化剂活性成分的钯和铂以1∶0.1~0.5的重量比浸渍。
2.如权利要求1所述的催化剂,其中,钯与铂的重量比为1∶0.1~0.3。
3.如权利要求2所述的催化剂,其中,所述催化剂具有陶瓷基质,所述陶瓷基质上沉积有选自氧化铝、氧化锆、二氧化硅、二氧化铈及其混合物的载体和作为催化剂活性成分的钯和铂。
4.如权利要求3所述的催化剂,其中,所述载体为氧化铝。
5.如权利要求4所述的催化剂,其中,所述用于处理柴油LNG双燃料机动车的废气的催化剂可以通过包括以下步骤的方法制造:
通过将氧化铝洗涂在陶瓷基质上制备经洗涂的基质,然后干燥并煅烧所述经洗涂的陶瓷基质;和
通过将所述经洗涂的基质浸入含有钯和铂的催化溶液中来浸渍催化剂活性成分,然后干燥并煅烧所述经洗涂的陶瓷基质。
6.如权利要求5所述的催化剂,其中,所述催化溶液包含H2PtCl6作为铂前体。
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RU2715732C2 (ru) | 2015-03-05 | 2020-03-03 | Шелл Интернэшнл Рисерч Маатсхаппий Б.В. | Катализатор окисления метана, процесс его получения и способ его применения |
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CN113042038A (zh) * | 2021-03-24 | 2021-06-29 | 中国科学院生态环境研究中心 | 一种钯铂催化剂、其制备方法及应用 |
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