CN105854553A - 一种吸收结合光电反应降解有害气体的方法及装置 - Google Patents
一种吸收结合光电反应降解有害气体的方法及装置 Download PDFInfo
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Abstract
一种吸收结合光电反应降解有害气体的方法及装置,特别涉及从气流中去除烃、醇、醛、醚、酚、酮、酯、胺、四氢呋喃和杂环化合物等挥发性有机物,硫化氢、硫氧化碳、一氧化氮和氨等无机物,该方法的处理过程是把含有害气体的气流导入吸收塔,其中的有害气体被吸收液和吸收液中的活性炭和光催化剂颗粒吸收和吸附后,吸收液连同活性炭和光催化剂颗粒被进一步导入光电反应器,在所述的光电反应器中,被吸收液和活性炭及光催化剂颗粒吸收和吸附的有害气体在铁碳微电解和光催化共同作用下被氧化和降解,最终把气流中的有害气体有效去除,从而达到气体净化的目的,吸收液、活性炭和光催化剂循环利用。
Description
技术领域
本发明涉及一种吸收结合光电反应降解有害气体的方法及装置,特别涉及从气流中去除烃、醇、醛、醚、酚、酮、酯、胺、四氢呋喃和杂环化合物等挥发性有机物,硫化氢、硫氧化碳、一氧化氮和氨等无机物的方法和装置,属于大气污染控制和环境保护技术领域。
背景技术
含烃、醇、醛、醚、酚、酮、酯、胺、四氢呋喃和杂环化合物等挥发性有机物的有害气体,以及硫化氢、硫氧化碳、一氧化氮和氨等无机物的有害气体,产生于化学、制药、喷漆和污水处理站等各种生产过程。这些污染物(包括恶臭气体),不仅对人体有害,有些还是致癌物质,而且大量排放还对区域环境产生了严重的影响。但是,由于这些气体或化学结构较稳定,不易降解,或阈值较低,给净化处理带来很大的困难。
一般地,采用水溶液吸收法是去除这些有害气体的主要方法之一,但此方法的主要问题是吸收容量有限,吸收液容易饱和。吸收后的溶液须进一步处理,如果直接送回废水池,被吸收处理后的产物又会挥发出来,将会导致二次污染的产生。如何在提高吸收效率的同时,又能降解这些污染物是该技术工业应用过程中急需解决的问题。
光催化技术作为一种新型的环境净化技术,一般以TiO2等N型半导体作为催化剂主体,其基本原理是在紫外光源照射下,TiO2价带中的电子就会越过禁带被激发到导带上,形成带负电的高活性电子,同时在价带上产生带正电的空穴,这些空穴可以将吸附在TiO2表面的OH-和H2O分子氧化成羟基自由基(OH),而羟基自由基能与污染物反应,将其最终降解为CO2和H2O等无害物质。但是,由于光生电子和空穴在内部以及表面的自主复合,抑制了光催化降解有害物的能量效率,因此如何提高光催化降解的效率成为该技术工业应有的关键课题之一。铁碳微电解法是处理难降解废水的一种处理方法,其原理利用铁屑与活性炭之间存在的电位差,在液相形成了无数个微小的原电池,在微电解过程产生的活性自由基能与污染物反应,最终把有害物转化为无害物。
本发明的目的是设计和提供一种溶液吸收结合光电反应的方法和装置,用于从气流中除去所述的有害气体,使气流中含有的这些有害气体得到有效吸收和降解,从而达到气体净化的目的。
发明内容
本发明采用的技术方案为:一种吸收结合光电反应降解有害气体的方法,其特征在于把含有害气体的气流导入吸收塔,其中的有害气体被吸收液和吸收液中的活性炭和光催化剂颗粒吸收和吸附后,吸收液连同活性炭和光催化剂颗粒被进一步导入光电反应器,在所述的光电反应器中,被吸收液和活性炭及光催化剂颗粒吸收和吸附的有害气体在铁碳微电解和光催 化共同作用下被氧化和降解,最终把气流中的有害气体有效去除,从而达到气体净化的目的,吸收液、活性炭和光催化剂循环利用。
本发明采用的吸收塔为通用的气液吸收设备如喷淋塔、填料塔、鼓泡塔、旋流板塔或筛板塔等,吸收液为水溶液,气液接触时间约1s以上,所述的有害气体为酸性时,吸收液一般为碱性,有害气体为碱性时,吸收液一般为酸性,就光电反应器而言,一般在酸性环境下更有利于微电解和光催化反应,优选pH为3-7,可通过添加盐酸、硫酸或磷酸等调整吸收液pH值,也可添加一定量的氯化钠或硫酸钠等盐作为电解质增加纯水的电导率,一般为10%以下。
本发明所述装置的吸收塔下部设置有气体进口,顶部设置有气体出口,底部设置有吸收塔循环水槽,吸收塔循环水槽通过循环水泵进液管、循环水泵和循环水泵出液管与吸收塔进液口连通,吸收塔出液口通过出液管与光电反应器连通,所述的光电反应器的中上部通过溢流回液管与吸收塔循环水槽连通,光电反应器底部设置有曝气管通入氮气或空气以带动铁粉、活性炭颗粒和光催化剂等物料在光电反应器内流化接触,形成流化床反应区,光电反应器的上部设置有回气管与吸收塔塔体连通,所述的光电反应器的上部还设置有紫外光源,所述的紫外光源一般设置在光电反应器的液面上方,铁粉、活性炭和光催化剂等固体颗粒通过光电反应器上部的药剂加入口加入光电反应器,所述的光电反应器还设置有排液口。
本发明所述的光电反应器一般为圆筒或方型结构,其中加入的铁质材料作为微电解的阳极,活性炭作为有害物的吸附剂和微电解的阴极,所述的铁质材料可采用铁粉,也可采用网状或规整填料充填,两种类型材料的处理效果相当,但添加铁粉较方便,下面以添加铁粉作为示例说明。选用的铁粉粒径以易于流化为宜,优选1mm以下,作为有害物的吸附剂和微电解的阴极的粉状活性炭颗粒,粒径小些较好,优选3mm以下,活性炭在液相的充填率(体积)一般为70%以下,优选1%-30%,作为微电解的电极对,铁碳理论摩尔比例一般为1∶1,活性炭颗粒又作为吸附剂,可适当过量,无特殊要求。所述的光催化剂一般采用P25型TiO2晶体,也可采用掺杂或改性处理的TiO2光催化剂和其他如ZnO、SnO2、ZrO2和WO3等光催化剂或混合物,效果大体相当,以TiO2稳定性好,具体可参看相关文献。以P25型TiO2光催剂为例,主要由锐钛型矿型和金红石型组成,以锐钛型矿型为主,光催化剂平均粒径小些为好,一般为500nm以下,优选10-50nm,添加量可根据催化剂颗粒大小、需处理的有害物和处理要求等参数选定,一般为0.1g/L(或液相有害物浓度10倍)以上,优选1g-30g/L。光源可采用高压汞灯等紫外光光源,光源波长范围200-500nm,具体可依据光催化剂特性选用,光源功率一般为1-5kW/m3,一般置于液面上方,吸收液在光电反应停留时间为10s以上,优选60s-3600s,具体可根据紫外光源功率、光催化剂量和吸收液中有害物浓度等参数确定,一般所述的有害物浓度低,反应时间可短,光源功率小,处理时间就相对较长。
所述的有害气体的吸收塔吸收与光电降解反应是一连续过程的两个操作单元步骤,其中活性炭和光催化剂颗粒随吸收液循环流动,在吸收塔内可起到吸附有害物的作用,同时活性炭和光催化剂在光电反应器内分别又作为微电解的电极和光催化剂参加反应,把铁碳微电解和光催化相结合,使得光生电子和空穴在光催化剂内部以及表面的自主复合大为减少,从而提高了光催化的降解效率。
所述的有害气体主要为烃、醇、醛、醚、酚、酮、酯、胺、四氢呋喃和杂环化合物等挥发性有机物,硫化氢、硫氧化氮、一氧化氮和氨等无机物的一种或几种。
本发明所述的光电反应器的底部还设置有曝气管向反应器内鼓入氮气或空气加强化学反应,使反应器中的铁粉、活性炭和光催化剂充分流化接触,最小曝气量应能使所有颗粒在反应器内流化,铁粉可依据消耗量或连续或定期加入,铁离子在吸收液中饱和后,可在吸收液中加入氢氧化钠后使铁沉淀或以离子交换等方式分离后,吸收液可循环使用。
本发明所述的光电反应器中还可加入一定比例的玻璃珠等光反射颗粒材料,工作时和铁粉和活性炭等固体颗粒一起处于流化状态,在光照下形成反射把光线反射到光催化剂表面,从而促进光化学反应。一般所述的玻璃珠等反光材料的颗粒直径一般小于5mm,优选0.5-2mm,流化量一般为光电反应器内吸收液量的20%以下,优选1-5%,也可在光电反应器内壁表面贴附反光材料,如树脂反光膜等来促进光化学反应,总体可提高降解率约5%。
与现有技术相比,本发明的优点在于:采用气液吸收和和光电反应相结合,使有害气体在吸收塔被吸收液和吸收液中的活性炭和光催化剂颗粒吸收和吸附,再通过铁炭微电解和光催化联合化学反应使有害物得到降解,从而提高了吸收效果和光催化反应的效率。
附图说明
图1为本发明所述的一种吸收结合光电反应降解有害气体方法的装置结构示意图,其中:1循环水泵;2循环水泵进液管;3吸收塔循环水槽;4加液口;5气体进口;6循环水泵出液管;7吸收塔进液口;8气体出口;9吸收塔塔体;10吸收塔出液口;11出液管;12回气管;13紫外光源;14溢流回液管;15药剂加入口;16光电反应器;17排液口;18曝气管。
所述的循环水泵1通过循环水泵出液管6与吸收塔进液口7连通,吸收塔出液口10通过出液管11与光电反应器16连通,光电反应器16上部设置有回气管12与吸收塔塔体9连通,光电反应器16中上部通过溢流回液管14与吸收塔循环水槽3连通,光电反应器16底部设置有曝气管18通入氮气或空气带动铁粉、光催化剂和活性炭等颗粒物料在光电反应器16内流化,中上部还设置紫外光源13,铁粉、光催化剂和活性炭等颗粒物料通过药剂加入口15加入光电反应器16,吸收塔循环水槽3通过循环水泵进液管2与循环水泵1连通,光电反应器16还设置有排液口18。
具体实施方式
以下结合附图实施例对本发明作进一步详细描述。
本发明所述的一种吸收结合光电反应器降解有害气体方法的装置如图1所示。吸收塔为填料塔,材质PP,塔径为Φ250mm,充填Φ25阶梯环,填料层高度约为1500mm。光电反应器为圆筒型,外形尺寸为Φ600mm×1500mm,立式放置。
处理工艺流程是待处理含有害气体的气流由进气口5进入吸收塔9内与喷淋液接触,进行吸收反应,处理后的气流从塔顶出气口8排出,吸收液通过吸收塔下部的出液管11进入光 电反应器17,接通紫外光源13,同时通过光电反应器17的下部设置的曝气管18向反应器内鼓入空气或氮气使物料流化,光电反应器17的上部有回气管12把曝气废气接回吸收塔9吸收,吸收液通过溢流回液管14返回出吸收液循环水槽3,经循环水泵1打回吸收塔9。
实验条件为:载气为空气,流量约120m3/h,。气液接触时间约3-5s,气体相对湿度约70%,气体温度约25℃;循环泵流量约1m3/h,气体浓度分析方法为气相色谱仪,稳定运行一小时后测定。氮气曝气量约为15L/min。初始吸收液为清水,加入量约500kg,加稀盐酸到pH为5左右。吸收液在光电反应器停留时间约为30min。
铁粉为含量98%,平均粒径约0.1mm,初期活性炭与铁粉摩尔比例为3∶1,活性炭粒径约为0.1mm,加入量约20kg。光催化剂采用P25型TiO2微晶体,其中锐钛型矿型和金红石型的组成比例约为8∶2,粒径约为20-30nm,比表面积约为50m2/g,加入光催化剂量约0.5kg。紫外光源采用1.5kW高压汞灯,置于反应器液面上方约15cm,光源波长范围200~400nm。
实验结果如表1所示。
表1有害物去除效果
有害物 | 进口浓度(mg/m3) | 出口浓度(mg/m3) |
二氯甲烷 | 251 | 45 |
甲苯 | 340 | 35 |
氯苯 | 201 | 35 |
苯乙烯 | 363 | 39 |
甲醇 | 392 | 21 |
甲硫醇 | 97 | 4 |
*** | 216 | 37 |
甲硫醚 | 157 | 35 |
二乙胺 | 89 | 5 |
环氧乙烷 | 226 | 33 |
甲醛 | 305 | 32 |
丙酮 | 368 | 27 |
甲酸乙酯 | 231 | 22 |
乙酸乙酯 | 250 | 23 |
四氢呋喃 | 120 | 10 |
硫化氢 | 80 | 4 |
氨 | 139 | 9 |
二硫化碳 | 276 | 29 |
一氧化氮 | 401 | 53 |
实施例2:光催化剂采用ZnO微晶体,其结构主要为六方纤锌矿型,粒径约为20-30nm,比表面积约为50m2/g,加入光催化剂量约1kg。吸收液pH约为6左右。在光电反应器加入液体体积比约1%的平均粒径为1mm的玻璃珠反光材料,工作时在反应器内和铁粉及催化剂一起处于流化状态,所述的光电反应器内壁表面还贴附有树脂反光膜,反射率约为70%。其他条件同实施例1。
实验结果:如表2所示。实验还发现当加入光催剂量降为0.1kg时,有害物平均去除率约降低10%左右。再增加催化剂加入量,有害物去处理率变化不大。
表2有害物去除效果
有害物 | 进口浓度(mg/m3) | 出口浓度(mg/m3) |
二氯甲烷 | 262 | 41 |
甲苯 | 351 | 32 |
氯苯 | 187 | 34 |
苯乙烯 | 386 | 35 |
甲醇 | 401 | 21 |
甲硫醇 | 102 | 4 |
*** | 237 | 38 |
甲硫醚 | 169 | 35 |
二乙胺 | 105 | 6 |
环氧乙烷 | 255 | 34 |
甲醛 | 310 | 28 |
丙酮 | 375 | 25 |
甲酸乙酯 | 263 | 24 |
乙酸乙酯 | 250 | 21 |
四氢呋喃 | 141 | 11 |
硫化氢 | 85 | 4 |
氨 | 146 | 6 |
二硫化碳 | 293 | 27 |
一氧化氮 | 385 | 51 |
应该说明的是,以上实施例仅用于说明本发明的技术方案,本发明的保护范围不限于此。对于本领域的技术人员来说,凡在本发明的精神和原则之内,对各实施例所记载的技术方案进行修改,或者对其中的部分技术特征进行任何等同替换、修改、变化和改进等,均应包含在本发明的保护范围之内。
Claims (10)
1.一种吸收结合光电降解有害废气的方法,其特征在于把待处理含有害气体的气流导入吸收装置,其中的有害气体被吸收液和吸收液中的活性炭和光催化剂颗粒吸收和吸附后,吸收液连同活性炭和光催化剂颗粒被进一步导入光电反应器,在所述的光电反应器中,被吸收液和活性炭及光催化剂颗粒吸收和吸附的有害气体在铁碳微电解和光催化共同作用下被氧化和降解,最终把气流中的有害气体有效去除,从而达到气体净化的目的,吸收液、活性炭和光催化剂循环利用。
2.根据权利要求1所述的方法,其特征在于所述的有害气体含烃、醇、醚、醛、酚、酮、酯、胺和有机物,硫化氢、硫氧化碳、一氧化氮氮和氨无机物的一种或几种。
3.根据权利要求1所述的方法,其特征在于所述的光催化剂包括TiO2、ZnO、SnO2、ZrO2和WO3,添加量为0.1g/L以上。
4.根据权利要求1所述的方法,其特征在于所述的吸收塔为通用的气液吸收设备喷淋塔、填料塔、鼓泡塔、旋流板塔或筛板塔。
5.根据权利要求1所述的方法,其特征在于所述的吸收液为pH为3-7的水溶液,通过添加盐酸、硫酸或磷酸调整吸收液pH值。
6.根据权利要求1所述的方法,其特征在于所述的光电反应器为圆筒或方型结构,其中装填有作为微电解阳极的铁质材料和作为有害物吸附剂和微电解阴极的活性炭;所述的铁质材料为网状或规整填料或铁粉,所述的铁粉粒径1mm以下,所述的活性炭粒径3mm以下,活性炭在液相的充填率为70%以下。
7.根据权利要求1或6所述的方法,其特征在于所述的光电解反应器的下部设置有曝气管向反应器内鼓入空气或氮气,并使反应器中的所有固体颗粒处于流化状态。
8.根据权利要求1或6所述的方法,其特征在于所述的光电反应器的紫外光源置于反应器内液面上方,光源波长范围为200-500nm,光源功率为1-5kW/m3,吸收液在光电反应停留时间为10s以上。
9.根据权利要求1或6所述的方法,其特征在于所述的光电反应器内加入溶液体积20%以下的玻璃珠反光材料,所述的光电反应器内壁表面还贴附有树脂反光膜。
10.根据权利要求1所述的一种吸收结合光电降解有害废气的方法的装置,其特征在于所述的装置包括吸收塔、吸收液循环水槽及光电反应器;所述的吸收塔下部设置有气体进口,顶部设置有气体出口,底部设置有吸收塔循环水槽,吸收塔循环水槽通过循环水泵进液管、循环水泵和循环水泵出液管与吸收塔进液口连通,吸收塔出液口通过出液管与光电反应器连通,光电反应器的上部设置有回气管与吸收塔塔体连通,光电反应器的中上部通过溢流回液管与吸收塔循环水槽连通,光电反应器底部设置有曝气管通入氮气或空气以带动铁粉、活性炭、光催化剂和玻璃珠等颗粒物料在光电反应器内流化,形成流化床反应区,所述的光电反应器的中上部液面上方还设置紫外光源,所述的铁粉、活性炭、光催化剂和玻璃珠等药剂可通过光电反应器上部的药剂加入口加入光电反应器,所述的光电反应器还设置有排液口。
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