CN111093808A - 进行焦炉烟道气的选择性催化还原的方法 - Google Patents
进行焦炉烟道气的选择性催化还原的方法 Download PDFInfo
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Abstract
本发明涉及在低温下对焦炉烟道气进行选择性催化还原(SCR)的方法,其中使用焦炉煤气(COG)作为还原剂,将其混合到烟道气中,并使用SCR催化剂。所使用的SCR催化剂可以是催化过滤袋或催化陶瓷过滤烛的形式,以同时去除颗粒和相关的催化剂毒物以及NOx和残余的氢和烃。
Description
技术领域
本发明涉及一种用于在低温下进行焦炉烟道气的选择性催化还原(SCR)的方法。
背景技术
SCR系统使用催化剂来促进烟道气NOx与还原剂之间的反应,所述还原剂通常为氨,其被注入到烟道气流中。用于该目的的催化剂选择性地将NOx转化为氮气和水,从而将NOx排放减少高达97%。
SCR是氮氧化物(NO和NO2)与氨的催化反应,以根据反应方案形成单质氮和水
4NO+4NH3+O2->4N2+6H2O
NO+NO2+2NH3->2N2+3H2O
6NO3+8NH3->7N2+12H2O
2NO2+4NH3+O2->3N2+6H2O
前两个反应是主要的反应,其中每转化一摩尔的NOx消耗一摩尔氨。后两个反应发生在气体中,其中大部分的NOx以NO2存在。为了在250-450℃范围内的温度下进行反应,使用催化剂。最常见的SCR催化剂类型是基于TiO2载体上的V2O5催化剂。
焦炉(coke oven)设备在NOx排放方面面临着越来越严格的法规,特别是在迄今为止是焦炭生产最大市场的中国。
在炼焦厂中,焦炭在焦炉中由煤来生产。在此,通过加热到900至1400℃的温度将煤中的挥发性成分热解,然后释放和提取。这形成焦炭,其基本上由碳和含有挥发性成分的废气组成,并且被称为炼焦厂气(coking plant gas)。在无氧的条件下在焦炉中进行热解。这原则上是间歇过程,并且释放的炼焦厂废气的组成波动。然而,由于总是操作多个焦炭收集器,所以平均气体组成仅经历小的波动。因此,所形成的炼焦厂气含有H2(约55%)、N2、CO2、硫和高级烃。
焦炉气(COG)是焦炭制造过程的副产物。COG由各种气体的复杂混合物组成。其组成通常由55%H2、6%CO、25%CH4(甲烷)加上小百分比的CO2(二氧化碳)、H2O(水分)、重质焦油、挥发性烃和硫杂质组成。它还含有一些N2(氮)。焦炉气中的高级烃、焦油和芳族化合物通常通过一系列冷却、冷凝和分离步骤从气流中提取。这种液体副产物是市售的,并且被称为焦炉焦油(coke oven tars),其在全世界范围内交易。COG通常表示来自这一系列该焦油提取处理步骤的剩余气体,并且通常用作炼钢厂内各种加热应用的燃料气体,并且过剩的COG用于产生蒸汽或电力,或者将其燃烧。使用COG生产直接还原铁(DRI)一直是令人感兴趣的,但是挑战是将甲烷转化为CO和H2以及清除焦油和挥发性烃。
通过燃烧COG的再生燃烧器提供用于焦炉熔炉(coke oven furnace)的热量。
焦炉气含有烃,例如BTX(苯、甲苯和二甲苯的三种异构体(o、m和p)的混合物)、甲烷、H2和CO。COG的处理和利用不仅提高了钢铁工业的能效,而且防止了包括CO2和甲烷在内的有害温室气体的排放。考虑到未来的氢经济,具有高氢含量的焦炉气具有巨大的工业和商业价值。目前,许多钢铁企业的目标是在钢铁制造过程中利用各种现场工艺中的气体的同时使其COG过剩最小化。尽管已经进行了广泛的研究和开发以利用过剩的COG,但是仍然浪费了大量的COG,导致生产效率低和严重的温室气体排放。
在现有技术中,焦炉气已经用于各种目的。因此,US4.270.739描述了利用含硫气体如焦炉气作为工艺气体直接还原铁氧化物的方法和设备。该方法特别适用于使用含有有机硫的气态工艺燃料。
WO2006/013455描述了一种用于从焦炉气中生产清洁的还原性气体的方法和装置,其中将衍生自煤的挥发性组分转化成适合用作合成气、用作铁矿石直接还原的还原剂和/或用作清洁燃料的还原性气体。
US2016/0083811描述了一种使用焦炉气将铁氧化物还原成金属铁的方法。该方法包括将焦炉气分成多个焦炉气流,将第一焦炉气流提供至氢富集单元以形成富氢产物流,将该富氢产物流作为还原性气流的一部分递送至还原竖炉,以及将尾气流从氢富集单元提供至重整反应器以形成重整气流,将该重整气流作为还原性气流的一部分递送至还原竖炉。任选地,净化来自还原竖炉的废炉顶气流中的CO2并将其再循环回还原性气流。
在US2012/0261244中,公开了一种用于从焦炉的废气中减少氮氧化物的方法。该方法包括燃烧可燃气体(其部分或全部地由焦炉气组成),以产生含有氮氧化物的烟道气。在700-1100℃下将还原剂,优选氨,加入到烟道气中,通过还原剂和氮氧化物之间的均相气体反应来还原烟道气中的氮氧化物组分,同时在再生器中从烟道气中回收热量。
CN107014217A公开了利用来自焦化装置的焦炉气和处理烟道气的系统和方法。具体地,它描述了一种通过在将焦炉烟道气通入SCR之前将其与焦炉气混合而对焦炉烟道气进行选择性催化还原的方法。尽管焦炉气在到达SCR之前通过锅炉,但是焦炉气的一部分必须保持未反应,以使焦炉气能够保持其还原能力,这意味着锅炉在亚化学计量条件下运行。
已经研究了在称为MidrexTM工艺的工艺中使用COG代替天然气作为还原剂来直接还原铁矿石(Kobelco Technology Review 33,pages 16-20,Feb.2015)。该方法在没有焦炭的情况下运行,排放较少的CO2,因此作为高炉炼铁的替代方法而受到关注。
COG可用于各种其它目的,例如用于氢分离的原料。目前,钢铁工业中的一些现场焦化厂使用变压吸附(PSA)从COG获得H2(Bermúdez et al.,Fuel Process Technol.110,pages 150-159,2013)。该方法在使用不同吸附材料如氧化铝或沸石的循环吸附-解吸操作中进行。COG重整还提供了一种较低能量密集型和更清洁的合成气生产的有吸引力的替代方案(Li et al.,Chem.Eng.Technol.30,pages 91-98,2007)。
来自焦炉燃烧的烟道气包含NOx(即NO和NO2)、SO2和颗粒物作为主要污染物。SO2排放的程度取决于焦炉气的脱硫程度。NOx排放的程度可通过低NOx燃烧技术来降低。
与来自炼焦厂的烟道气排放的气体控制相关的挑战在于,烟道气在低温下离开再生加热/冷却块。热耗尽的烟道气含有二氧化硫(SO2),因此当氨用作还原剂时,形成硫酸氢铵,因此催化剂快速失活成为问题。因此,本发明的构思是用焦炉气代替通常使用的氨作为还原剂。
发明内容
因此,本发明涉及一种用于在低温下对焦炉烟道气进行选择性催化还原(SCR)的方法,其中
-焦炉气用作还原剂,将其混合到烟道气中,和
-使用SCR催化剂。
此外,所使用的SCR催化剂可以是催化过滤袋或催化陶瓷过滤烛的形式,以同时去除颗粒和相关的催化剂毒物以及NOx和残余的氢和烃。此外,甲醇和/或DME可以单独使用或与焦炉气组合使用。
通过使用基于氧化钒和钯的催化剂来氧化逃逸组分,可以减轻H2、CO和BTX的逃逸。这将提供一种非常有效的手段来减少炼焦厂中的NOx。
低工艺温度优选为100-250℃,更优选150-230℃,最优选170-210℃。
Claims (7)
1.一种用于在低温下对焦炉烟道气进行选择性催化还原(SCR)的方法,其中
-焦炉气用作还原剂,将其混合到烟道气中,和
-使用SCR催化剂。
2.根据权利要求1所述的方法,其中使用基于在TiO2载体上的钯和V2O5的催化剂。
3.根据权利要求1或2所述的方法,其中所使用的SCR催化剂是催化过滤袋或催化陶瓷过滤烛的形式,以同时去除颗粒和相关的催化剂毒物以及NOx和残余的氢和烃。
4.根据权利要求1或2所述的方法,其中所使用的SCR催化剂是催化过滤袋或催化陶瓷过滤烛的形式,并且注入SOx吸附剂以同时除去SOx、颗粒和相关的催化剂毒物以及NOx和残余的氢气和烃。
5.根据前述权利要求中任一项所述的方法,其中所述温度为100-250℃。
6.根据权利要求5所述的方法,其中所述温度为150-230℃。
7.根据权利要求6所述的方法,其中所述温度为170-210℃。
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