CN110821625A - 一种船舶发动机尾气后处理净化系统 - Google Patents
一种船舶发动机尾气后处理净化系统 Download PDFInfo
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Abstract
本发明公开了一种催化协同低温等离子体脱除PM和NOx船舶尾气后处理净化系统，尤其适用于采用柴油为燃料动力的船舶、固定源柴油动力发电机组等尾气净化处理。该系统将催化剂协同低温等离子体脱除碳烟颗粒(PM)及NOx，该系统由氧化型催化单元，等离子体发生器，氧化型颗粒半通透式过滤器以及选择性还原催化单元组成，并按照先后顺序进行集成，含催化剂的催化单元孔目数在20目～100目之间，氧化型颗粒半通透式过滤器的璧孔隙率≥50％。整个系统背压低，快速净化PM和NOx，PM捕集率大于90％，脱除效率大于95％，NOx转化效率≥95％。
Description
技术领域
本发明属于尾气净化技术领域，尤其属于发动机尾气催化净化技术领域，特别涉及一种船舶发动机尾气后处理净化系统。
背景技术
柴油发动机具有燃油经济性高、可靠性强、动力大、寿命长等优势，被广泛用于汽车、轮船、固定源发电机组、海上石油平台柴油发电机等大型设备上。但是，柴油机尾气污染也给人类生存环境造成了极大的威胁。柴油机尾气主要包括水蒸气、O2、N2、CO和CO2、碳氢化合物(HC)、氮氧化合物(NOX)、硫化物及颗粒污染物(PM)，颗粒污染物主要包括碳烟粒子、高可溶性碳氢、铅化物等，其中氮氧化合物(NOX)和颗粒污染物(PM)是造成柴油机尾气污染的主要成分。
针对船舶、海上石油平台等大型柴油发电机尾气有害排放物对大气造成的潜在危害，已受到IMO(国际海事组织)、MEPC(国际环保委员会)及其它机构和各国政府的高度重视，并已制定了一些严格的排放措施来限制船舶对大气的污染。
目前，船舶已成为我国沿海、沿河地区主要的大气污染源。相对与港口来说，我国内河航运线上的污染情况要更为复杂，我国内河船舶约22万余艘，2000多万载重吨，大多船型旧，吨位小，根据计算，我国内河船舶每年排放大气的NOx、SOx约不少于100万吨，随着MARPOL73/78公约附则Ⅵ第三阶段标准的实施和我国船舶大气污染物排放法规、标准的不断完善，开展船舶大气污染控制迫在眉睫。
针对船舶尾气的净化，目前比较主流的技术方案是废气净化系统(EGC)，搭配SCR-DeNOx净化，综合了开发式和混合式的优点，通过使用海水洗涤废气(对海水碱度有要求)和添加NaOH或MgO的海水加淡水洗涤废气，可实现污水零排放，实现废气脱硫效果好，相当于燃用含硫量0.1％的燃油，PM脱除率可达80％，船舶依然可以燃用含硫量为3.5％的重油，船舶运营成本低。但是也伴随着一些缺点，首先就是SCR反应器及洗涤塔体积较大，布置难度高，要是针对在用船的改造，难度将非常大，同时对柴油机背压影响较大，一般都需要加装风机，成本也非常高。
根据目前对PM的捕集及其脱除方式而言，一方面采用柴油颗粒过滤器进行过滤，通过气流反吹进行物理吹扫，或者采用燃烧器进行外加热，实现直接燃烧，这些都会带来很多弊端，一方面是吹扫不彻底，碳烟会很快聚集，导致背压快速增加，另一方面通过燃烧器加热，能耗高，当聚集大量的碳烟，进行直接燃烧时，过滤器芯部温度可能急剧增加，导致不安全，另一种方式是通过催化氧化法，在一定温度条件下，将碳烟与NO2发生氧化还原反应，通常要求温度280℃～500℃，要求有足够的NO2量，当在280℃以下时，催化能力不够，碳烟的氧化脱除效率低，当船舶发动机长期在较低负荷下运行时，会急剧造成碳烟排放，且背压急剧增加。与之同时，船舶通常要求背压低于10kPa，这会要求柴油碳烟颗粒过滤器体积很大，相应地，占用船舶大量空间，部分船舶无法进行合理的布局安装，因此都不能较广泛的应用。
发明内容
本发明根据现有技术的不足及其排放进化要求，公开了一种催化协同低温等离子体脱除PM和NOx船舶尾气后处理净化系统。本发明要解决的问题是提供一种多级催化单元，经过优选的催化材料，合适的低温等离子体发生器配型，同时搭配SCR进行优化集成，形成一个完整的尾气净化系统，实现PM和NOx的同时去除，尤其是实现较低温度下的PM净化，实现整个系统低背压要求，因此尤其适合对PM和NOx的船舶等尾气的净化。
本发明通过以下技术方案实现：
船舶发动机尾气后处理净化系统，设置于船舶发动机尾气排放端通道，其特征在于：依次由氧化型催化单元(DOC)、低温等离子体发生器(NTP)、氧化型颗粒半通透式过滤器(POC)和选择性还原催化单元(SCR)顺序构成。
所述系统各单元孔目数是20目～200目，氧化型颗粒半通透式过滤器的璧孔隙率≥50％，PM捕集率大于90％，脱除效率大于95％，NOx净化效率≥95％，温度活性窗口为100℃～500℃。
所述氧化型催化单元包括催化材料和贵金属制成的气体通透结构的处理器；催化材料为无机多孔陶瓷粉体材料的混合物，贵金属包括铂和钯，其中：重量比Pt:Pd＝1:0～5:1，贵金属总含量5～10g/ft3。
所述催化材料包含氧化硅、氧化铝、氧化钛组成的复合氧化物，其他组分包含单相氧化物或/和复合氧化物，单相氧化物包括：氧化锆、氧化铈、氧化镧、氧化镨；复合氧化物包括：氧化铝-氧化硅、氧化铝-氧化锆、氧化铝-氧化钛、氧化铈-氧化锆、氧化铈-氧化镨，氧化铝-氧化铈、氧化铝-氧化镧、氧化铝-氧化镨；其他组成包含以上的一种或以上。主成分质量含量≥95％，其他组分质量含量≤5％，含主成分的复合氧化物与其他成分的氧化物之间，是相互独立的催化材料种类。
所述低温等离子体发生器采用高压脉冲供电方式产生等离子体，频率范围：50～300HZ，电压范围：10～100kV。
所述氧化型颗粒半通透式过滤器催化剂涂层采用铈基复合金属氧化物制成，其中氧化铈质量含量≥90％，助剂添加物质量含量≤10％；催化剂涂层还通过贵金属铂，贵金属总含量0.1～2.0g/ft3。
所述氧化型颗粒半通透式过滤器材质为金属材质，氧化型颗粒半通透式过滤器截面孔隙率大于50％。
所述选择性还原催化单元所述选择性还原催化剂涂覆材料为钛硅钨复合氧化物：其质量含量比例是：五氧化二钒1％～5％，氧化钨5％～15％，二氧化钛80％～94％。
本发明采用催化协同低温等离子体脱除PM和NOx船舶尾气后处理净化系统，净化系统包括氧化型催化单元(Diesel Oxidation Catalyst,DOC)，低温等离子体发生器(Non-thermal Plasma,NTP)，氧化型颗粒半通透式过滤器(Partical oxidation catlytic,POC)以及选择性还原催化单元(Slective Catalyst reduction,SCR)。
系统能够同时协同净化碳烟颗粒(PM)和氮氧化合物(NOx)，实现系统背压低的要求。
本发明氧化型催化单元+等离子体发生器+氧化型催化颗粒半通透式过滤器+选择性还原催化单元进行集成。按照此顺序对各个组件进行组装，以实现催化协同等离子体脱除PM和NOx双降目的。
本发明氧化型催化单元，用于去除HxC，CO，同时对NO进行氧化，产生NO2，低温等离子体发生器用于对废气流进行激发、电离、离解，产生氧化能力极强的活性粒子OH＊，HO2＊，O＊，O3等，同时辅助提到NO氧化为NO2，氧化型颗粒半通透式过滤器用于过滤PM，同时将其净化，催化氧化为CO2，选择性还原催化单元用于去除NOx，将其转化为N2，PM捕集效率大于90％，脱除效率大于95％，NOx脱除效率≥95％。
针对DOC催化层反应包括：NO+O2→NO2(温度：200℃～500℃)
本发明系统将DOC至于NTP发生器前端，将本发明的催化剂涂覆在DOC载体内孔道表面上，催化材料中包含贵金属，在200℃以下，即可以将发动机涡后排除的HC和CO废气进行净化干净，同时对部分NO进行氧化，生成NO2，随着废气流进入到NTP发生器之中，在高压电压脉冲情况下，对废气流中的气体进行激活，产生大量的具有极强氧化性的粒子，主要包含O*、OH*、HO2 *、O3等，同时对气流中部分NO进行氧化，产生NO2，在NTP发生器中产生的活性粒子，原位发生氧化还原反应，将PM进行氧化，产生CO2，随着废气流的传输，进入下游的POC净化器之中，进一步对未处理的PM进行过滤，同时发生氧化还原发生，主要是NO2作为氧化剂，与之同时，在POC的过滤层上面涂覆含贵金属的催化剂，能将废气流中的NO进行氧化，产生NO2，协助上游中已有的NO2，一起对捕集到的PM进行氧化净化，最终实现高效捕集与净化的目的，将此过程称为“两级捕集与净化”。在NTP发生器中发生的PM氧化，在低至100℃时候，就能实现，这主要是因为NTP发生器产生的活性粒子氧化能力强，这为整个系统实现较低温度的净化能力奠定基础。在POC中,NO2与PM发生反应，温度在260～500℃就可以发生良好的氧化反应，最终整个系统在100～500℃之间，具有良好的PM捕集和净化能力。
结合低温等离子体净化效率高,能耗低以及无二次污染等特点，对碳烟进行低温净化，有效地拓宽碳烟氧化温度，同时在催化剂协助之下，满足在整个发动机运行工况的温度区间范围，即100℃～500℃温度范围内，对碳烟的有效净化。
根据低温等离子体对碳烟氧化的可能途径包括：
1)C+2O*→CO2
2)C+4OH*→CO2+2H2O
3)3C+4HO2 *→3CO2+2H2O
4)3C+2O3→3CO2
通过以上途径，将产生的具有极强氧化性粒子与PM发生氧化反应，且在较低温度下就能发生，一般低至100℃，就有30％以上的氧化效率。
相应地，还对NO具有氧化能力，及氧化性粒子与NO发生反应，生成大量的NO2，由于NO2也具有较强的氧化性能，也将进一步地与PM发生反应，结合上游DOC产生的大量的NO2，在经过低温等离子体净化PM后，在POC中，经捕集的PM进一步在较高温度下发生反应，从而协同实现PM的净化，最终实现95％的脱除率。
NTP协助NO发生氧化反应，产生NO2包括：
1)NO+O*→NO2
2)NO+2OH*→NO2+H2O
3)NO+HO2 *→NO2+OH
4)3NO+O3→3NO2
在POC催化层中的反应包括：
NO+O2→NO2(温度：200℃～500℃)
DOC、POC与NTP产生的大量的NO2协同氧化PM：
2NO2+C→2NO+CO2(温度：100℃～500℃)
随着废气流通过POC过滤器之后，进入下游的SCR催化器，在SCR催化器入口端喷射尿素，使经过雾化后的尿素液与废气流进行充分混合，再经过SCR反应器床层，在催化剂作用下，NH3与NOx发生氧化还原后，净化为N2，实现NOx净化。
针对SCR催化层反应包括：
1)4NH3+4NO+O2→4N2+6H2O，标准SCR反应：NO占90％，富氧，300～400℃；
2)2NH3+NO2+NO→2N2+3H2O，快速SCR反应：NO2增加，NO:NO2＝1:1最佳；
3)8NH3+6NO2→7N2+12H2O，SCR缓慢反应：多余NO2参与发生反应。
在还原剂NH3的参与下，经过快SCR反应，能实现95％以上的NOx净化效率。
在实际运行过程中，对POC前后端的背压进行监测，当显示背压高于预警值时，则启动NTP发生器，以便在较低温度下就进行PM的氧化净化，同时辅助提高POC中的PM净化，使整个系统背压被控制在一个安全范围内。在SCR前后端安装NOx传感器，根据传感器反馈的NOx浓度信息，进行尿素含量的喷射，使在SCR反应器中的催化还原反应始终处于快SCR反应路径进行，实现良好的NH3利用及其NOx的净化。
附图说明
图1是本发明催化系统布置示意图。
图中，F是发动机，ΔP是压力传感器，A是NOx传感器，T1是第一温度传感器，T2是第二温度传感器，DOC是氧化型催化单元，NTP是低温等离子体发生器，POC是氧化型颗粒半通透式过滤器，SCR是选择性还原催化单元，各箭头方向是气体流动方向。
具体实施方式
下面结合具体实施方式对本发明进一步说明，具体实施方式是对本发明原理的进一步说明，不以任何方式限制本发明，与本发明相同或类似技术均没有超出本发明保护的范围。
结合附图。
以下实施例DOC贵金属总量为5g/ft3，所用白载体是堇青石材料的蜂窝陶瓷载体(35目/in2),所用半通透式POC目数100目/in2。
实施例1
一种催化协同低温等离子体脱除PM和NOx船舶尾气后处理净化系统，包括如下步骤：
按照本专利要求对DOC采用Si-Al-Ti/CeO2材料做催化剂，将贵金属浸渍到材料中，其中贵金属摩尔比Pt:Pd＝3:1，形成DOC催化剂并涂覆于35目蜂窝陶瓷载体中，对NTP采用100HZ，对POC过滤器采用Ce-Ti复合材料，其中二氧化钛质量含量5％,贵金属为单Pt；针对SCR催化剂，五氧化二钒，氧化钨和二氧化钛三种材料进行复合，其质量含量分别为3％，10％和87％。最终实现PM过滤效率为92％，PM脱除效率为95％，NOx转化效率为96％。
实施例2
一种催化协同低温等离子体脱除PM和NOx船舶尾气后处理净化系统，包括如下步骤：
按照本专利要求对DOC采用Si-Al-Ti/Al-Ce材料做催化剂，将贵金属浸渍到材料中，形成DOC催化剂并涂覆于35目蜂窝陶瓷载体中，对NTP采用150HZ，对POC过滤器采用Ce-Ti复合材料，其中二氧化钛质量含量5％，针对SCR催化剂，五氧化二钒，氧化钨和二氧化钛三种材料进行复合，其质量含量分别为5％，5％和90％。最终实现PM过滤效率为94％，PM脱除效率为95％，NOx转化效率为97％。
实施例3
一种催化协同低温等离子体脱除PM和NOx船舶尾气后处理净化系统，包括如下步骤：
按照本专利要求对DOC采用Si-Al-Ti/Ce-Zr材料做催化剂，将贵金属浸渍到材料中，形成DOC催化剂并涂覆于35目蜂窝陶瓷载体中，对NTP采用300HZ，对POC过滤器采用Ce-Ti复合材料，其中二氧化钛质量含量5％，针对SCR催化剂，五氧化二钒，氧化钨和二氧化钛三种材料进行复合，其质量含量分别为5％，10％和85％。最终实现PM过滤效率为96％，PM脱除效率为97％，NOx转化效率为97％。
附表1为各具体实施案例所获得PM过滤效率、脱除效率及其NOx的转化效率。
表1：性能统计表
| PM过滤效率 | PM脱除效率 | NOx转化效率 | |
| 实施例1 | 92％ | 95％ | 96 |
| 实施例2 | 94％ | 95％ | 97 |
| 实施例3 | 96％ | 97％ | 97 |
表2发动机排放信息
通过对NTP的脉冲调整及其合理的DOC，POC和SCR催化剂匹配，最终实现对PM的整体过滤效率达到90％及以上，PM的脱除效率达到95％以上，以及对NOx转化效率达到95％以上。在低温等离子协同催化转化情况下，实现了船舶尾气PM和NOx共同净化。
附1：检测方法描述，具体如下：
将形成的后处理各部件，进行组装后，对系统末端采用烟度计进行PM透光度检测，以确定对PM的捕集效率，当检测结束之后，对系统中的POC进行称重，直接检测未被脱除的PM重量，最终确定PM的脱除效率，在POC两端安装压差及温度传感器，检测碳烟捕集对压差的影响。在SCR反应器入出口端安装NOx传感器，检测系统两端NOx含量，确认NOx的转化效率。
Claims (7)
1.一种船舶发动机尾气后处理净化系统，设置于船舶发动机尾气排放端通道，其特征在于：依次由氧化型催化单元、低温等离子体发生器、氧化型颗粒半通透式过滤器和选择性还原催化单元顺序构成。
2.根据权利要求1所述的船舶发动机尾气后处理净化系统，其特征在于：所述系统各单元孔目数是20目～200目，氧化型颗粒半通透式过滤器的璧孔隙率≥50％，PM捕集率大于90％，脱除效率大于95％，NOx净化效率≥95％，温度活性窗口为100℃～500℃。
3.根据权利要求2所述的船舶发动机尾气后处理净化系统，其特征在于：所述氧化型催化单元包括催化材料和贵金属制成的气体通透结构的处理器；催化材料为无机多孔陶瓷粉体材料的混合物，贵金属包括铂和钯，其中：重量比Pt:Pd＝1:0～5:1，贵金属总含量5～10g/ft3。
4.根据权利要求2所述的船舶发动机尾气后处理净化系统，其特征在于：所述低温等离子体发生器采用高压脉冲供电方式产生等离子体，频率范围：50～300HZ，电压范围：10～100kV。
5.根据权利要求2所述的船舶发动机尾气后处理净化系统，其特征在于：所述氧化型颗粒半通透式过滤器催化剂涂层采用铈基复合金属氧化物制成，其中氧化铈质量含量≥90％，助剂添加物质量含量≤10％；催化剂涂层还通过贵金属铂，贵金属总含量0.1～2.0g/ft3。
6.根据权利要求5所述的船舶发动机尾气后处理净化系统，其特征在于：所述氧化型颗粒半通透式过滤器材质为金属材质，氧化型颗粒半通透式过滤器截面孔隙率大于50％。
7.根据权利要求2所述的船舶发动机尾气后处理净化系统，其特征在于：所述选择性还原催化单元所述选择性还原催化剂涂覆材料为钛硅钨复合氧化物：其质量含量比例是：五氧化二钒1％～5％，氧化钨5％～15％，二氧化钛80％～94％。
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| CN112682127A (zh) * | 2021-01-26 | 2021-04-20 | 太原科技大学 | 一种汽车尾气净化装置 |
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