CN112870939B - 一种用于连续有效去除空气污染物的生物耦合催化反应体系 - Google Patents
一种用于连续有效去除空气污染物的生物耦合催化反应体系 Download PDFInfo
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Abstract
本发明提供了一种用于连续有效去除空气污染物的生物耦合催化反应体系,属于环境污染控制和能源利用技术领域。反应体系包括光电催化耦合微生物燃料电池反应系统,气体溶解系统以及电催化耦合微生物系统。负载有催化剂的碳毡作为光电阴极,微生物与碳棒组合在一起形成阳极室,阳极室中的碳棒与光电阴极通过外部绝缘的铜线经过外部电阻连接以形成电路。在外加光源的条件下,光催化剂会产生大量电子空穴对,同时在微生物作用下协同降解污染物。系统可采用循环运行方式,生物阳极和水处理EC‑MFC连通起来,充分利用微生物的降解能力,达到更加的降解效果。
Description
技术领域
本发明属于环境污染控制中VOCs去除及能源利用技术领域,涉及Ag/AgBr/TiO2-ZnO纳米复合催化剂、光电催化功能组件的制备,耦合微生物和光电催化协同作用降解污染物且产生电能,采用循环系统充分利用微生物对VOCs的降解能力,用于连续去除乙酸乙酯和异丙醇,有助于提高空气质量,这对开发有效的环境修复技术来解决环境问题有着非常重要的意义。
背景技术
挥发性有机化合物(VOCs)是空气中最有害的污染物之一,会产生严重的环境问题,如雾霾,光化学烟雾,臭氧消耗和全球变暖。工业生产中排放的VOCs成分复杂,存在许多会给人体带来直接危害的物质,长时间吸入VOCs将会产生协调作用失衡、神经系统疲劳甚至丧失记忆的病症。随着工业的发展,生产过程中排放到大气中的VOC在逐渐增多。VOC是光化学烟雾的重要前体,能与大气中的羟基自由基(•OH)、氮氧化物(NOx)等发生光化学反应,导致地面烟雾的形成;还可以引起气候变暖,病态建筑综合征,植物腐烂和人类致癌等,所以加强VOC的污染控制和高效治理刻不容缓。而加强VOC污染控制,一方面需要研发高效催化材料,提高净化处理效率,另一方面加强耦合技术研究,促进节能和资源化。
微生物燃料电池(MFC)可以通过微生物氧化溶解的有机物直接发电。细菌产生的电子从阳极流向阴极,并与质子和氧结合形成水。UV辅助的光电耦合微生物燃料电池可用于废气净化,该系统将膜分离、光催化与MFC技术相结合来去除空气中的VOC同时发电。在这种的反应器中,阳极室充满了外生电子,并配备了中空室PVDF/CFC膜组件作为VOCs富集扩散层,负载在活性炭纤维毡基材上的CeO2/TiO2催化剂(CeO2/TiO2/ACF)合成为催化空气光电阴极。微生物可以通过接收来自气态底物(如甲醇)的电子并被终端电子受体氧(在有氧呼吸中)捕获来获得能量。当电子受体不是氧气,例如硝酸盐时,一些厌氧微生物能够利用来自气态供体的电子并将它们转移到硝酸盐中。因此,气态物质也可用于为MFC中的阳极微生物提供营养。但是现有研究的光电耦合微生物燃料电池(PEC-MFC)体系并没有充分的发掘利用微生物的降解能力。
发明内容
本发明的目的是通过对传统的光电催化耦合微生物燃料电池体系进行改进,充分利用微生物的降解能力,实现体系降解较高浓度VOCs的能力。成功构建了光电催化体系(PEC)、光电催化耦合微生物燃料电池体系(PEC-MFC)、单循环电催化耦合微生物燃料电池体系(C-EC-MFC)和单循环光电催化耦合微生物燃料电池体系(C-PEC-MFC),并分别对乙酸乙酯和异丙醇进行处理研究。为了降解溶解液中的乙酸乙酯和异丙醇,以及充分利用微生物的降解能力,成功构建了双循环电催化耦合微生物燃料电池体系(CC-EC-MFC)和双循环光电催化耦合微生物燃料电池体系(CC-PEC-MFC)。
本发明的技术方案:
一种用于连续有效去除空气污染物的生物耦合催化反应体系,主要由光电催化耦合微生物燃料电池反应系统、电催化耦合微生物系统和溶解系统三部分组成;
所述的光电催化耦合微生物燃料电池反应系统分为两个阴极室和一个阳极室,阴极室与阳极室间通过质子交换膜分隔开,两个阴极室间通过管路联通;阴极是由负载在碳毡上的催化材料构成,并靠于质子交换膜上;阳极由附着希瓦氏产电菌的活性炭组成;阳极与阴极间连接有外电阻;紫外灯位于两个阴极室外侧,照射到阴极上;
所述的电催化耦合微生物系统从下到上分为阳极室、沸石层和阴极室;阳极由附着希瓦氏产电菌的活性炭组成,阴极为碳毡,阳极和阴极间连接外电阻;
所述的溶解系统为一个密闭容器,其上连接有进气管、出气管、进水管和出水管;进气管用于向溶解系统中通入VOCS气体,出气管与光电催化耦合微生物燃料电池反应系统的阴极室相通,用于向其中通入VOCS气体;进水管分为两个管路,一个管路与光电催化耦合微生物燃料电池反应系统的阳极室相连,光电催化耦合微生物燃料电池反应系统阳极室出水进入到溶解系统中,另一个管路与电催化耦合微生物系统的出水管相连;出水管分为两个管路,一个管路与光电催化耦合微生物燃料电池反应系统的阳极室相连通,另一个管路与电催化耦合微生物系统的阳极室相连通;光电催化耦合微生物燃料电池反应系统的阴极室设有气体出口管路。
所述的催化材料是Ag/AgBr/TiO2-ZnO纳米复合光催化剂,催化剂经过溶胶凝胶法和光还原法制的。
所述的外电阻控制为10~10000Ω。
所述的VOCS气体是可溶解于水中的,具体为乙酸乙酯和异丙醇。
本发明的有益效果:本发明提供了用于连续有效去除空气污染物的生物耦合催化反应体系,该体系实现光电催化和微生物的耦合,耦合装置净化效果明显且稳定,同时可以产电,实现在常温条件下降解VOC;通过将乙酸乙酯和异丙醇溶解在去离子水中并循环到EC-MFC系统和PEC-MFC系统,充分的利用微生物降解能力。
附图说明
图1为耦合装置示意图。
图2不同外部电阻下PEC-MFC体系对EA的降解效果。反应器两侧的阴极Ag/AgBr/TiO2-ZnO(100mg)作为催化剂。坐标为时间,单位分钟(min),纵坐标为降解率(%)。
图3不同的体系对乙酸乙酯降解的影响,图3(a)和3(b)分别为乙酸乙酯浓度1800mg/m3和异丙醇1620mg/m3时,催化剂在不同体系条件下对污染物的降解率曲线。横坐标为时间,单位分钟(min),纵坐标为降解率(%)。
具体实施方式
以下结合技术方案和附图详细说明本发明的具体实施方式。
一种用于连续有效去除空气污染物的生物耦合催化反应体系,气体进口流量为120ml/min,两侧各有一个紫外灯功率为5w为反应提供光照,负载有催化剂的碳毡与微生物燃料电池组合在一起形成PEC-MFC膜组件,由丙烯酸玻璃制成的反应器,微生物负载在活性炭上。阳极室体积为80cm3(5cm×8cm×2cm),内部容积为26.4cm3(2.4cm×5.5cm×2cm),负载有光催化剂的碳毡(2.4cm×5.5cm)作空气阴极,中间由PEM分离。外部用丙烯酸玻璃材质的中空隔板,橡胶垫和螺栓固定,隔板尺寸为5cm×8cm(中空部分为2.4cm×5.5cm),以保证不锈钢网和PEM充分接触,并且微生物阳极室不漏水。污染物可以更好地与催化剂接触,另一方面,少量的乙酸乙酯气体可以透过PEM和碳毡阳极室中用于微生物降解。微生物阳极通过碳棒(长度8cm,截面直径0.3cm,用橡胶塞固定)传导电子并通过铜线连接到阴极,外部电路接有电阻,经电流表和电压表测量观察相应的电流和电压变化。PEC-MFC阳极室和EC-MFC阳极室中的主要微生物菌株是实验室储存的厌氧产电菌(希瓦氏产电菌)。
EC-MFC系统主要用于降解溶解在去离子水中的乙酸乙酯和异丙醇。反应器总体积为2L,系统由下至上分别为阳极微生物层、沸石隔离层和阴极层。阳极层主要是由负载有产电菌的活性炭组成,体积为800ml,沸石隔离层的体积为700ml,采用碳毡做空气阴极,阴极层体积为500ml。溶有乙酸乙酯和异丙醇的溶解液由反应器底部进入到EC-MFC体系,自下而上经过阳极微生物层、沸石隔离层和阴极层,然后处理过的液体循环到气体溶解系统中。
阴极的制备:取一定量的催化剂粉末于玻璃片上,滴加适量硅胶溶液,形成悬浮液,均匀涂覆到碳毡(选用3cm×8cm的碳毡),用硅胶溶液涂覆有效面积为13.2cm2(2.4cm×5.5cm)将涂好的电极材料放入烘箱中60℃进行干燥,备用。
阳极的制备:微生物(希瓦氏产电菌)附着在颗粒状活性炭上,碳棒用于收集和传导电子。
实施例1
结合图1,首先气体经过溶解系统,经过去离子水吸收后的乙酸乙酯和异丙醇进入PEC-MFC系统,流量计控制流速为120mL/min-125mL/min。含有乙酸乙酯和异丙醇吸收液分别循环到PEC-MFC系统和EC-MFC系统的阳极室,PEC-MFC系统和EC-MFC系统的阳极室的出水流回溶解系统。在测量污染物的浓度时同时采用万用表记录外电阻R两端的电压。其中光电阴极制备过程如下:
通过溶胶-凝胶法制备TiO2-ZnO纳米材料。首先,将0.68gZnSO4溶解在36mL蒸馏水和80mL甲醇的混合物中,搅拌后,用氨水将溶液的pH调节至9。然后,向混合物中滴加20mL钛酸丁酯并搅拌3 h以形成白色溶胶。将溶胶在75℃下搅拌并加热,得到白色粉末,然后将样品在温度为80℃条件下真空干燥2 h,并在马弗炉中以5℃/min的加热速率在510℃下煅烧2h。冷却至室温后,收集浅黄色产物并研磨成粉末。
通过离子交换和光还原过程依次合成Ag/AgBr/TiO2-ZnO化合物。首先,将1 g制备的TiO2-ZnO充分分散在30 mL去离子水中,加入适量的AgNO3,在将溶液搅拌30 min后,将20ml NaBr溶液逐滴添加到溶液中。反应1小时后,用去离子水彻底洗涤,得到AgBr/TiO2-ZnO悬浮液。然后在磁力搅拌下用9W紫外灯照射溶液1h。用去离子水和乙醇洗涤催化剂,离心三次。将离心产物在60℃下干燥过夜。
实施例2
结合图1,采用图1中的PEC-MFC系统降解乙酸乙酯,反应开始每隔20min,进行取样测定,不同电阻降解图如图2,电阻变化范围10Ω-10000Ω。
实施例3
结合图1,采用图1中的装置,图3(a)和(b)分别为乙酸乙酯浓度1800 mg/m3和异丙醇1620mg/m3时,催化剂在不同体系条件下对污染物的降解率曲线。PC系统:材料加光照。EC系统:阳极室加入0.5M电解质溶液,插入铜棒,外接电阻构成回路。PEC系统:加光照,阳极室加入0.5M电解质溶液,插入碳棒。EC-MFC系统:在EC系统基础上将阳极室0.5M电解质溶液替换为微生物。C-EC-MFC:溶解液体循环到PEC-MFC系统不加光照。C-PEC-MFC:溶解液体循环到PEC-MFC系统加光照。
Claims (5)
1.一种用于连续有效去除空气污染物的生物耦合催化反应体系,其特征在于,该生物耦合催化反应体系主要由光电催化耦合微生物燃料电池反应系统、电催化耦合微生物系统和溶解系统三部分组成;
所述的光电催化耦合微生物燃料电池反应系统分为两个阴极室和一个阳极室,阴极室与阳极室间通过质子交换膜分隔开,两个阴极室间通过管路联通;阴极是由负载在碳毡上的催化材料构成,并靠于质子交换膜上;阳极由附着希瓦氏产电菌的活性炭组成;阳极与阴极间连接有外电阻;紫外灯位于两个阴极室外侧,照射到阴极上;
所述的电催化耦合微生物系统从下到上分为阳极室、沸石层和阴极室;阳极由附着希瓦氏产电菌的活性炭组成,阴极为碳毡,阳极和阴极间连接外电阻;
所述的溶解系统为一个密闭容器,其上连接有进气管、出气管、进水管和出水管;进气管用于向溶解系统中通入VOCS气体,出气管与光电催化耦合微生物燃料电池反应系统的阴极室相通,用于向其中通入VOCS气体;光电催化耦合微生物燃料电池反应系统的另一个阴极室设有气体出口管路;进水管分为两个管路,一个管路与光电催化耦合微生物燃料电池反应系统的阳极室相连,光电催化耦合微生物燃料电池反应系统阳极室出水进入到溶解系统中,另一个管路与电催化耦合微生物系统的出水管相连;出水管分为两个管路,一个管路与光电催化耦合微生物燃料电池反应系统的阳极室相连通,另一个管路与电催化耦合微生物系统的阳极室相连通。
2.根据权利要求1所述的用于连续有效去除空气污染物的生物耦合催化反应体系,其特征在于,所述的催化材料是Ag/AgBr/TiO2-ZnO纳米复合光催化剂,催化剂经过溶胶凝胶法和光还原法制的。
3.根据权利要求1或2所述的用于连续有效去除空气污染物的生物耦合催化反应体系,其特征在于,所述的外电阻控制为10~10000Ω。
4.根据权利要求1或2所述的用于连续有效去除空气污染物的生物耦合催化反应体系,其特征在于,所述的VOCS气体是可溶解于水中的。
5.根据权利要求3所述的用于连续有效去除空气污染物的生物耦合催化反应体系,其特征在于,所述的VOCS气体是可溶解于水中的。
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