CN103052446B - 适于轻油成分的燃烧的氧化催化剂 - Google Patents
适于轻油成分的燃烧的氧化催化剂 Download PDFInfo
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Abstract
本发明的目的在于提供氧化催化剂(DOC),其即使在耐久后,也适于使在柴油颗粒过滤器(DPF)再生时供给的轻油成分在比较低的温度下燃烧,其耐热性和耐久性优异。而且,适于轻油成分的燃烧的本发明的氧化催化剂(DOC)具有以水银孔隙率测定计测定的细孔分布的峰值为10~100nm的范围内的氧化铝多孔体、和担载于该氧化铝多孔体的表面上和/或细孔内壁面上的贵金属。另外,本发明的氧化催化剂(DOC)构成体为在含陶瓷或金属材料的催化剂支持体上担载前述氧化催化剂(DOC)。
Description
技术领域
本发明涉及适于轻油成分的燃烧的氧化催化剂,特别涉及下述氧化催化剂(以下记为DOC),其可与柴油颗粒过滤器(以下记为DPF)一起安放于柴油发动机的排气气体流路内,配置于DPF的更上游侧,使在DPF的再生时供给的轻油成分在比较低的温度下燃烧。
背景技术
在柴油发动机的排气气体中含有微粒(颗粒),微粒的大部分由煤和可溶性有机物质构成,是形成环境污染的原因,因此它的除去处理是重要的。
为了防止微粒被排放到大气中,有效的是在排气气体流路内设置DPF来捕集微粒。但是,随着微粒的捕集,DPF会发生堵塞,导致产生排气阻力,因此,为了消除该堵塞,需要除去被捕集的微粒以进行DPF的再生。
DPF中捕集的微粒在氧的存在下加热至高温(约600℃以上)时,发生自燃从而可容易地除去。但是,通常,仅依靠排气气体的热量时温度的上升并不充分,非常难以使微粒完全燃烧而消除DPF的堵塞。因此,为了消除DPF的堵塞,现有技术中提出了各种方法或手段。
已知为了使DPF强制再生而将轻油等燃料供给到排气气体中,通过DOC使之燃烧而形成高温气体,由此使DPF中捕集的微粒燃烧的方法(例如,参照专利文献1~4),提出了可使轻油在比较低的温度下燃烧的各种DOC(例如,参照专利文献2~4)。
现有技术文献
专利文献
专利文献1:日本特开平8-312331号公报
专利文献2:日本特开2004-290827号公报
专利文献3:日本特开2007-315274号公报
专利文献4:日本特开2009-228575号公报。
发明内容
发明要解决的技术问题
现有使用的DOC可在耐久前的初期在比较低的温度下使轻油燃烧,但在耐久后,可使轻油燃烧的温度存在上升的趋势。因此,本发明的目的在于提供:即使在耐久后,也适于使在DPF再生时供给的轻油成分在比较低的温度下燃烧,耐热性和耐久性优异的DOC。
用于解决技术问题的方法
本发明人等为了实现上述目的而进行了深入研究,结果发现,使贵金属担载于以水银孔隙率测定计测定的细孔分布的峰值在特定的范围内的氧化铝多孔体而成的DOC,即使在耐久后,也能使在DPF再生时供给的轻油成分在比较低的温度下燃烧,从而完成了本发明。
即,本发明的适于轻油成分的燃烧的DOC,其特征在于,具有以水银孔隙率测定计测定的细孔分布的峰值为10~100nm的范围内的氧化铝多孔体、和担载于该氧化铝多孔体的表面上和/或细孔内壁面上的贵金属。
另外,本发明的适于轻油成分的燃烧的DOC构成体,其特征在于,具有含陶瓷或金属材料的催化剂支持体、和担载于该催化剂支持体的上述本发明的适于轻油成分的燃烧的DOC。
发明效果
本发明的适于轻油成分的燃烧的DOC和DOC构成体,即使在耐久后,也适于使在DPF再生时供给的轻油成分在比较低的温度下燃烧,耐热性和耐久性优异。
附图说明
[图1]显示实施例1~6和比较例1中使用的各La稳定化θ氧化铝的以水银孔隙率测定计测定的细孔分布的图。
具体实施方式
以下,详细地说明本发明。
本发明的适于轻油成分的燃烧的DOC,具有以水银孔隙率测定计测定的细孔分布的峰值为10~100nm的范围内的氧化铝多孔体、和担载于该氧化铝多孔体的表面上和/或细孔内壁面上的贵金属。
本发明中使用的氧化铝多孔体,以水银孔隙率测定计测定的细孔分布的峰值为10~100nm,优选为20~60nm,更优选为30~55nm的范围内。使用以水银孔隙率测定计测定的细孔分布的峰值小于10nm的氧化铝的DOC时,由于耐久后的DOC的作用,能使轻油成分燃烧的温度(燃点)变得比较高,作为DOC在实用上是不充分的。对于使用了以水银孔隙率测定计测定的细孔分布的峰值大于100nm的氧化铝的DOC,由于耐久后的DOC的作用,能使轻油成分燃烧的温度(燃点)变得如何并不明确。
在本发明中,可使用α氧化铝、γ氧化铝、θ氧化铝等各种氧化铝的多孔体。对于氧化铝多孔体的比表面积,优选为100~200m2/g左右。另外,优选使用La稳定化(经La2O3稳定化的)氧化铝多孔体。在该La稳定化氧化铝多孔体中,Al2O3/La2O3的质量比优选为99/1~93/7,更优选为97/3~95/5。
由下述的实施例、比较例也明显可知,在本发明的适于轻油成分的燃烧的DOC中,优选使用以水银孔隙率测定计测定的细孔分布的峰值为10~100nm范围内的La稳定化氧化铝多孔体,更优选使用20~60nm范围内的La稳定化氧化铝多孔体,进一步优选使用30~55nm范围内的La稳定化氧化铝多孔体。通过使用具有这种细孔分布的峰值的La稳定化氧化铝多孔体,由于耐久后的DOC的作用,能使轻油成分燃烧的温度(燃点)仍为比较低的状态。
使用以水银孔隙率测定计测定的细孔分布的峰值为10~100nm范围内的氧化铝多孔体时,即使在该氧化铝多孔体的表面上和/或细孔内壁面上担载贵金属,例如选自Pt、Pd、Rh、Ag、Au、Ru和Ir中的至少1种贵金属,由于耐久后的DOC的作用,能使轻油成分燃烧的温度(燃点)也比较低。但是,优选担载选自Pt、Pd和Rh中的至少1种贵金属。
本发明的适于轻油成分的燃烧的DOC在柴油发动机的排气气体流路内使用时,可制为担载于由陶瓷或金属材料构成的催化剂支持体的状态的DOC构成体使用。DOC的担载量优选为30~250g/L,更优选为50~200g/L。另外,作为贵金属的担载量,优选为1~4g/L,更优选为1.5~3.5g/L。在这样的本发明的DOC构成体中,含陶瓷或金属材料的催化剂支持体的形状没有特别的限定,一般截面形状为矩形、三角形、蜂窝状等的连通的单元的集合体,陶瓷泡沫、金属丝筛网、金属发泡体、板、颗粒等形状,优选为蜂窝形状。另外,作为这样的催化剂支持体的材质,例如,可列举氧化铝(Al2O3)、莫来石(3Al2O3-2SiO2)、堇青石(2MgO-2Al2O3-5SiO2)、碳化硅(SiC)等陶瓷、或不锈钢等金属材料。
在本发明的DOC构成体中,作为氧化促进材料的ZrO2、CeO2等,或作为HC吸附材料的沸石、硅酸盐等多孔材料等可与上述DOC一起担载并混合存在。另外,还可以使作为氧化促进材料的ZrO2、CeO2等,或作为HC吸附材料的沸石、硅酸盐等多孔材料等担载于由陶瓷或金属材料构成的催化剂支持体而形成层,在该层上担载DOC而进行多层化。
在本发明的DOC构成体中,除氧化铝多孔体中10~100nm范围内的细孔分布的峰值之外,也存在在凝集粒子间形成的500nm以上的细孔分布的峰值。
本发明适于轻油成分的燃烧的DOC,特定地,可与DPF一起安放于柴油发动机的排气气体流路内,配置在DPF的更上游,使在DPF的再生时供给的轻油成分在比较低的温度下燃烧。
作为DPF,也可以使用任何公知的DPF。另外,也可以使用催化剂化的DPF。例如,可使用在堇青石等多孔陶瓷上涂布氧化铝等,进而担载了Pt、Pd、Rh等贵金属的DPF。
对排气气体流路中的轻油的供给,可在排气气体流路设置轻油喷射阀,并由此喷射经调节的量的轻油。
通过本发明的DOC而燃烧并形成高温气体,可将含有轻油的排气气体供给至DPF,使DPF堆积的微粒燃烧汽化而除去。由此,将DPF再生。
实施例1~6和比较例1
混合具有以水银孔隙率测定计测定的在第1表中记载的各种细孔分布的峰值、含有4质量%的La2O3且比表面积为150m2/g的任意一种La稳定化θ氧化铝多孔体180g,氧化铝浓度20质量%的氧化铝溶胶100g和纯水320g,并向其中加入规定量的二硝基二氨合铂水溶液和硝酸钯水溶液,搅拌30分钟以制备催化剂涂布用浆料。将该浆料涂布在直径143.8mm、长度76.2mm的堇青石制蜂窝基材(300孔/平方英寸、壁厚8mm)上,用鼓风除去多余的浆料。接着在120℃下干燥3小时,进而在空气中在500℃下烧成1小时。对于得到的DOC构成体,每1升堇青石制蜂窝基材涂布有100g的催化剂。其中Pt的担载量为1.6g/L,Pd的担载量为0.4g/L。
实施例1~6和比较例1中使用的各La稳定化氧化铝的以水银孔隙率测定计测定的细孔分布如图1所示。
对于实施例1~6和比较例1中得到的初期(未耐久处理)的DOC构成体和在电炉中750℃下耐久处理100小时的DOC构成体,使用实机发动机排气气体按下述方法测定轻油开始燃烧的温度(燃点)。
在将2.4L的装有涡轮的柴油发动机的转速固定为1050rpm的状态下,使连接发动机的动力计的负荷改变,使DOC构成体入口的排气气体温度为任意温度。在各温度下喷雾0.97L/h的JIS2号轻油5分钟,通过测定DOC构成体出口的排气气体温度来判断燃烧性。将确认到燃烧的、DOC构成体入口的排气气体温度的最低温度作为燃点。测定结果如第1表所示。
[表1]
由第1表所示的数据明显可知,使用了以水银孔隙率测定计测定的细孔分布的峰值为10nm以上的氧化铝多孔体的本发明的DOC构成体中,即使在750℃下耐久处理100小时后,相对于轻油的着火性能也优异。
Claims (9)
1.适于轻油成分的燃烧的氧化催化剂,其特征在于,具有以水银孔隙率测定计测定的细孔分布的峰值为10~100nm的范围内的氧化铝多孔体、和担载于该氧化铝多孔体的表面上和细孔内壁面上的贵金属。
2.根据权利要求1所述的适于轻油成分的燃烧的氧化催化剂,其使用了以水银孔隙率测定计测定的细孔分布的峰值为30~55nm的范围内的氧化铝多孔体。
3.根据权利要求1所述的适于轻油成分的燃烧的氧化催化剂,其中,氧化铝多孔体为La稳定化氧化铝多孔体。
4.根据权利要求2所述的适于轻油成分的燃烧的氧化催化剂,其中,氧化铝多孔体为La稳定化氧化铝多孔体。
5.根据权利要求1所述的适于轻油成分的燃烧的氧化催化剂,其中,贵金属为选自Pt、Pd和Rh中的至少1种。
6.根据权利要求2所述的适于轻油成分的燃烧的氧化催化剂,其中,贵金属为选自Pt、Pd和Rh中的至少1种。
7.根据权利要求3所述的适于轻油成分的燃烧的氧化催化剂,其中,贵金属为选自Pt、Pd和Rh中的至少1种。
8.根据权利要求4所述的适于轻油成分的燃烧的氧化催化剂,其中,贵金属为选自Pt、Pd和Rh中的至少1种。
9.适于轻油成分的燃烧的氧化催化剂构成体,其特征在于,具有含陶瓷或金属材料的催化剂支持体、和担载于该催化剂支持体的权利要求1~8中任一项所述的适于轻油成分的燃烧的氧化催化剂。
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