CN1198960A - 选择性还原废气中氮氧化物的方法 - Google Patents

选择性还原废气中氮氧化物的方法 Download PDF

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CN1198960A
CN1198960A CN98107034A CN98107034A CN1198960A CN 1198960 A CN1198960 A CN 1198960A CN 98107034 A CN98107034 A CN 98107034A CN 98107034 A CN98107034 A CN 98107034A CN 1198960 A CN1198960 A CN 1198960A
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P·肖布耶
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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/18—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control
    • F01N3/20—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control specially adapted for catalytic conversion ; Methods of operation or control of catalytic converters
    • F01N3/2066—Selective catalytic reduction [SCR]
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B01D53/9404—Removing only nitrogen compounds
    • B01D53/9409—Nitrogen oxides
    • B01D53/9431—Processes characterised by a specific device
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
    • F01N3/28—Construction of catalytic reactors
    • F01N3/2892—Exhaust flow directors or the like, e.g. upstream of catalytic device
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2610/00—Adding substances to exhaust gases
    • F01N2610/02—Adding substances to exhaust gases the substance being ammonia or urea
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/10—Internal combustion engine [ICE] based vehicles
    • Y02T10/12—Improving ICE efficiencies

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  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • Combustion & Propulsion (AREA)
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Abstract

本发明涉及在温度为200—600℃的废气中选择性催化还原NOx的方法,包括步骤(a)通过雾化喷嘴将含能还原NOx的还原剂和/或其前体物的液滴雾喷入管道中;(b)使带有各液滴的废气流过气体管道中数组平行板叠片中的各板之间的空间,其中,第一组叠片板相对气体管道壁成大约45°角,第二组叠片板与第一组叠片板成90°且与气体管道壁成45°角,第三组叠片板与第一组叠片板平行,这样迫使气流以“之”字形的流动方式通过各组叠片板;(c)在通过最后一组叠片板后,使气体通过一层整体催化剂,以便由带有与管道壁平行的通道的还原剂对NOx进行还原。

Description

选择性还原废气中氮氧化物的方法
本发明涉及利用通过分解诸如尿素、尿素的水溶液或NH3的水溶液等化合物而获得的NH3对一般包含于柴油发动机排出的废气中的NOx进行选择性还原的方法，在所谓的SCR催化剂上游气相中用NH3对NOx进行选择性还原。
作为还原剂的化合物以喷嘴中形成的液体喷雾形式，被喷射到进行NOx催化还原过程通常所要求的温度为300-400℃的废气气流中。但是在NH3可被用作NOx还原过程的SCR催化剂之前，雾状液滴必须经过蒸发，且尿素必须分解成NH3、CO2和H2O。液滴的蒸发和分解大量吸热，因此液滴的蒸发和分解(气化作用)的速度受到热从热气体通过液滴四周的气雾向液滴表面传递的速度所限制。这就是说，液滴气化的时间t(滞留时间)可通过下述等式进行估算：
t＝k*d-2(T-Tmin)秒
式中，d为液滴的(初始)直径；T为气体温度，Tmin为可在适当速度下分解尿素所需的最低温度(即大约180℃)，而k则为与气体速度无关的常数。
因此，液滴的滞留时间随液滴大小的变化而稳定增加。
另外，喷嘴与SCR催化剂之间使气流中液滴完全气化所要求的距离与管道中的气流速度成比例增加。
据实验和计算估计废气中尿素浓度为35％的溶液的100μm溶液液滴，在300℃温度时，滞留时间为1秒左右，也就是说喷嘴与SCR催化剂之间的距离需要20m才能满足管道中气流速度为20m/s的液滴的完全气化。如果喷嘴与SCR催化剂之间的距离只有0.5m(正如柴油车的情况一样)，液滴直径则必须降至小于8μm，才能使SCR催化剂上游气相中的液滴完全气化。但这是非常困难的。
当整个催化块中的催化剂均是直道单体的催化块时，气流中大部分粒子或液滴通过SCR催化剂时不发生反应。
现已发现，如果使各油滴可与简便地安装在喷嘴与SCR催化剂之间的有限距离处(如柴油车)的物体的表面发生撞击，则由简单喷嘴生成的相对较大的还原剂液滴就能够快速且完全气化。
该物体的原理于附图1中示出。该物体由大量连续的叠片组构成，每一组叠片组由各平行板构成，该些平行板使得气体在不同组板之间的空间中呈“之”字形流动，因而液滴在流向每一次发生变化时均与板面发生撞击。当液滴撞击时，其表面溅破，由于几方面的理由各板被气体加热的效率高得多，因此液体以气相比以液滴形式可按高得多的速度被加热。因此，板加大了液体与气体之间热传导的表面积，并且，气雾对各滞留板和气体之间的热传递的限制比对沿气流被迫移动的液滴的限制高得多。
液滴与叠片板面撞击的趋势随液滴大小的增加，随板间的空间中气流速度的增加，按流动方向沿叠片板长从一组叠片板流到另一组叠片板的气流偏转角度的增加以及各组叠片中板间距离的减小而增加。附图2所示为经计算得出的气体中直径分别为20，50和100μm的液滴的流动轨迹，该气体流过3组按板间距离为10mm设置的各组叠片板，并且气体偏转90°角从一组叠片板流到另一组叠片板，且在叠片空间气流速度为8m/s。可以看出，100μm的液滴在流经第一组叠片时就已发生碰撞，50μm的液滴在流经第三组叠片后发生碰撞，而20μm的液滴通过全部三组叠片而未发生碰撞。
当一组板的位置相对另一组相邻板的位置产生位移致使在气体流向如图3所示的下一组叠片时板与板之间的空间被减小一半时，撞击效率将有所增加。
气化速度，以及特别是获得还原剂完全气化所需的气体最低温度，能够通过将诸如Al、Fe、Ti、Zr、Si、Zn和/或Mg氧化物之类的并用于催化分解的尿素材料涂覆在板表面或至少是板的撞击部分上而分别升高或降低。
气体的撞击和混和可以原则上通过将各板以与现有固定混合器同样的方式交错排列而相互结合。然而，当与气体混和相互结合后，因为气体在固定通道间的迂回撞击效果将降低，这样在某一混和效果时即会减小气体偏转。
气流通道的结构也可象图4所示那样通过叠加波纹垂直于管壁的波纹板材来代替图1所示的由多层平板构成的锐缘通道。在由波纹板之间的空间构成的通道中，气流大体上将以与图1所示上述排列的各平板间的空间中所形成的锐缘通道同样的方式偏转。

Claims (7)

1.在温度为200-600℃的废气中选择性催化还原NOx的方法，其包括以下步骤：(a)通过雾化喷嘴将含有能够还原NOx的还原剂和/或其前体物的液滴雾
喷入管道中；(b)使带有各液滴的废气流过气体管道中数组平行板叠片中的各板之间
的空间，其中，第一组叠片板相对气体管道壁成大约45°角安置，
第二组叠片板与第一组叠片板成大约90°且与气体管道壁成45°角
安置，第三组叠片板与第一组叠片板平行，这样迫使气流以“之”
字形的流动方式通过各组叠片板；(c)在通过最后一组叠片板后，使气体通过一层整体催化剂，以便由带
有与管道壁平行的通道的还原剂对NOx进行还原。
2.根据权利要求1的方法，其特征在于：全部液滴实际上均与各组叠片板中的各板壁相撞击，液滴直径大于临界直径，以此临界直径，每当气流方向转向而流经各组叠片板中的通道时，都造成液滴与上述管道壁进行碰撞。
3.根据权利要求2的方法，其特征在于：液滴直径大于20μm，由平行板构成的叠片板组数为1-10组，板与板之间的空间中的气流速度为2-30m/s，板间距离为3-50mm，每块板的长度为板间距离的1-5倍，相邻两组叠片板间的角度为50-140°。
4.根据权利要求1的方法，其特征在于：板是金属物质的，优选是由耐酸不锈钢合金构成。
5.根据权利要求1的方法，其特征在于：板由陶瓷材料，优选堇青石构成。
6.根据权利要求1的方法，其特征在于：板上覆有涂层，暴露于液滴撞击的表面至少应覆有0.01-1mm的涂层，涂层中至少含有Al，Fe，Ti，Zr，Si，Zn或Mg的氧化物中的一种。
7.根据权利要求1的方法，其特征在于：还原剂是带有重量百分比为30-100％的尿素与水的混合溶液。
CN98107034A 1997-03-13 1998-03-12 选择性还原废气中氮氧化物的方法 Pending CN1198960A (zh)

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US6074619A (en) 2000-06-13
EP0864732B1 (en) 2003-02-26
ATE233368T1 (de) 2003-03-15
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CA2231987A1 (en) 1998-09-13
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